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Abstract
Förster resonance energy transfer (FRET) and Auger recombination in quantum dots (QDs)-molecules system are important mechanisms for affecting performance of their optoelectronic and photosynthesis devices. However, exploring an effective strategy to promote FRET and suppress Auger recombination simultaneously remains a daunting challenge. Here, we report that FRET process is promoted and Auger recombination process is suppressed in CdTe/CdS QDs-Rhodamine101 (Rh101) molecules system upon compression. The greatly improved FRET is attributed to the shortened donor-acceptor distance and increased the number of molecules attached to QDs induced by pressure. The reduced Auger recombination is ascribed to the formation of an alloy layer at the core/shell interface. The FRET can occur 70 times faster than Auger recombination under a high pressure of 0.9 GPa. Our findings demonstrate that high pressure is a robust tool to boost FRET and simultaneously suppress Auger recombination, and provides a new route to QDs-molecules applications.
© 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
1. Introduction
Quantum dots (QDs)-molecules system has been a focus of intense research in the past two decades for applications ranging from light-emitting diodes (LEDs) and optical amplifiers to lasing, photovoltaics and solar energy conversion [1–3]. For the development and optimization of such applications, it is crucial to understand the photophysics and photochemistry of dynamic process [4–11], particularly fluorescence resonance energy transfer (FRET) and Auger recombination [12–14]. The FRET process has been shown to effectively enhance the performance of light-sensing and -harvesting functions [15–16]. In contrast to FRET process, the Auger recombination process loses energy in the form of heat, and is responsible for efficiency roll-off at QD-based applications [17–20]. Thus, fast FRET process, coupled with the slow Auger recombination process, are the crucial events associated with the efficiency and functionality of applications.
In recent years, significant efforts have been made in developing efficient approach to accelerate FRET process [21,22] and suppress the unwanted Auger recombination [23,24]. According to the Förster theory, the FRET requires an appreciable spectral overlap of acceptor absorption and the donor emission spectra, and is highly sensitive to the donor–acceptor separation distance and the number of adsorbed acceptor per QD [25,26]. Prior studies suggested that the FRET rate would be enhanced by varying the length of the linker molecule (bridge), assembling multiple acceptors on the surface of the QDs, or increasing acceptor concentration [27–31]. For suppressing Auger recombination of QDs, efficient ways are to increase the core volume or to smooth the confinement potential between core and shell materials [12,32–33]. Other approach such as engineering alloyed core-shell interface in the QDs has also been proposed to suppress Auger recombination [23,34]. The above results show that the FRET process can be well promoted, and Auger recombination can be effectively inhibited, respectively. However, up to date, simultaneously accelerating FRET process and suppressing the unwanted Auger recombination have not been achieved, which impedes applications of carrier-muliplication-enhanced photovoltaics and electrically pumped lasers [19,35]. Thus, developing a new strategy to simultaneously improve FRET and suppress Auger recombination in QDs-molecules system remains urgent.
Here, we present a new strategy to simultaneously facilitate the FRET process and suppress Auger recombination in the CdTe/CdS QDs-rhodamine101 (Rh101) molecules system by a facile high-pressure tool. By compressing the system from 1atm to 0.9Gpa, pressure shortened the donor-acceptor distance and increased the number of molecules attached to QDs, enhancing the FRET rate dramatically. Meanwhile, the strengthened formation of the alloy layer at core/shell interface of QDs upon compression lead the Auger recombination rate decrease rapidly. The femtosecond transient absorption (TA) experiments [36–38] reveal that the FRET rate is 7.1${\times} $ 109 S-1 under atmospheric pressure (1atm) and 1.7${\times} $ 1011 S-1 as pressure increasing to 0.9 GPa. The FRET rate can be accelerated for over 20 orders of magnitude. Meanwhile, the Auger recombination rate can be decreased 2-fold simultaneously. Furthermore, the FRET process occurs 70 times faster than Auger recombination process at 0.9 GPa. The FRET with a rate that exceeds Auger recombination process, suggest a great progress in fundamental science and in applied fields, including the development of efficient LEDs and reduced threshold optical gain media [39].
2. Experimental details
2.1 Materials
CdTe/CdS QDs and Rh101 molecules were purchased from Xingzi New Material (China) and Sigma (America) without further purification, respectively. The QDs-Rh101 complexes were obtained through adding Rh101 into QDs in aqueous solution. The QDs donor and Rh101 acceptor were solved in water to a concentration of 1 × 10−6 M and 5 × 10−6 M respectively. The surface ligand on the QDs is the 3-mercaptopropionic acid, which makes QDs dissolve well in water.
2.2 High-pressure generation
The diamond anvil cell (DAC) was carried out to generate pressure. The sample and ruby were packed into a DAC chamber with 800 μm diameter, constructed from a T301 steel gasket with a thickness of 100 μm. Then a hole with 500 μm diameter was drilled in center of the indentation by the laser drilling machine. The pressure values were calibrated by the standard ruby fluorescent technique.
2.3 Spectroscopic measurements
The absorption spectra of the CdTe/CdS QDs and Rh101 molecule were obtained on the UV 2550 UV-vis spectrophotometer. The steady-state emission spectra of the CdTe/CdS QDs and QDs-Rh101 complexes were measured by the RF5301 fluorescence spectrophotometer. The femtosecond TA measurements were carried out via a power of 4 W at a 1 kHz repetition rate and 50 fs pulse width. The 400 nm pump pulse (3.1 eV pulse) were generated by Coherent Legend (50 fs, 1 kHz, 800 nm) regenerative amplifier with a BBO crystal. The excitation energy of the sample resolved pump pulses attenuation to 4 μJ. The white light continuum probe pulse was used to generate by a sapphire plate (HELIOS, Ultrafast Systems, United States). The pump pulse and probe pulse were combined in a spectrometer (HELIOS). The kinetic traces were fitted by using Surface Xplorer 2.2 Ultrafast Systems.
3. Results and discussion
Satisfying the basic requirement for the occurrence of FRET process, there is a good spectral overlap between CdTe/CdS QDs fluorescence and Rh101 molecules absorption in aqueous solution (Fig. 1(a)). The transmission electron microscope image of QDs is shown in Fig. S1 of Supplement 1. The absorption spectrum of QDs-Rh101 complexes is shown in Fig. 1(b). Then, we measured the fluorescence spectrum of QDs-Rh101 complexes in aqueous solution. Table S1 shows the emission intensity of QDs alone and QDs in the presence of Rh101 at different pressures. The addition of Rh101 causes a quenching in the fluorescence intensity of QDs. When compressing the QDs-Rh101 complexes from atmospheric pressure (1atm) to 0.9 GPa, the fluorescence quenching degree of QDs gradually increases (Fig. 1(c)). Furthermore, in addition to the emission quenching of QDs in the complexes, a new emission peak is formed at 623 nm, which is attributed to FRET-mediated Rh101 fluorescence. As increasing pressure from 1atm to 0.9Gpa, the ratio of Rh101 emission intensity to QDs emission intensity gradually increase (Fig. 1(d)), indicating the high pressure facilitate energy transfer from QDs donor to Rh101 acceptor.
Fig. 1. (a) Normalized absorption (Abs) and photoluminescence (PL) spectra of QDs donor and Rh101 dye acceptor measured with 400 nm excitation. (b) Absorption spectrum of QDs-Rh101 complexes. (c) Fluorescence (Flu) spectra of QDs-Rh101 complexes under high pressure from 1atm to 0.9G. (d) The ratio of Rh101 fluorescence intensity (F623 nm) to QDs fluorescence intensity (F516 nm) upon compression.
Furthermore, we recorded the chromaticity coordinates of QDs-Rh101 complexes emission under high pressure from 1atm to 0.9Gpa (Fig. 2(a)) [40]. Based on CIE chromaticity diagram, the emission of QDs-Rh101 complexes at 1atm lies to the green (0.33, 0.52) and its corresponding color temperature is in the range of 5000-6000 K. As increasing pressure from 1atm to 0.9Gpa, the emission colors of the QDs-Rh101 complexes change from green to yellow. In addition, Fig. 2(b) shows fluorescent images of QDs-Rh101 complexes. The change of luminescence colors of QDs-Rh101 complexes is consistent with the CIE chromaticity diagram. The luminescence color changing is derived from the pressure-enhanced FRET from QDs donor to Rh101 acceptor. Thus, we indeed developed high pressure as a powerful tool to facilitate the FRET process, along with the change in the chromaticity of emission in the QD-molecule system. The color tunability of the QDs-molecules system permits the development of light source with different luminosity characteristics for applications, particularly military navigation marker lights, where illumination specifications need to be regulated on demand.
Fig. 2. (a) Pressure-dependent chromaticity coordinates of the emissions of QDs-Rh101 complexes. (b) The fluorescent images (dark background) of QDs-Rh101 complexes at 1atm, 0.4Gpa and 0.8Gpa.
To expound the FRET process and Auger recombination process, the time-resolved TA spectroscopic measurements were carried out to track the real-time dynamics of the QDs-Rh101 system [41,42]. Figure 3(a,b) show time-resolved changes of the absorption ($\mathrm{\Delta }$ A) signals for QDs alone and QDs-Rh101 complexes in aqueous solution. Above-band gap excitation at 400 nm results in “bleaching” of ground-state populations in QDs alone and QDs-Rh101 complexes, shown as negative ${\Delta }$ A signals in Fig. 3(a,b) at 533 nm. In addition, an obvious difference between QDs alone and QDs-Rh101 complexes in the spectra at same delay time occurs (Fig. 3 (c,d)). Addition of Rh101 acceptor at short femtosecond time period does not change the transient absorption response, but changes the response over long delay time $( > $ 100ps) gradually. As delay time increased from 100ps to 2 ns, a new peak occurs at 584 nm (Fig. 3(d)), which should be ascribed from the FRET-induced appearance of absorption signals at a higher energy of bleach. Furthermore, to probe the FRET with temporal resolution, the TA kinetic traces of QDs alone and QDs–Rh101 complexes with global analysis are shown in Fig. 3(e). The two temporal constant by applying double-exponential decays are obtained in QDs alone system. Combining the previous study of QDs, the shorter lifetime (0.31ps) is attributed to the carrier relaxation process, and the longer lifetime (198.27ps) is derived from Auger recombination process [36,43,44]. Similarly, the three temporal constants for QDs–Rh101 complexes were recorded with three-exponential decays. In the QDs–Rh101 complexes, a new time scale in hundreds picoseconds appears (130.26ps), which comes from the FRET from the QDs donor to the Rh101 acceptor. Figure 3(f) schematically illustrates the FRET process between QD donor and Rh101 acceptor and Auger recombination process of QDs. For highly excited QDs, Auger recombination process consumes the energy of light-excited exciton (electron-hole pair), which subsequently loses this energy in the form of heat. The FRET process results in the exciton to migrate from QDs donor to Rh101 acceptor state and induces emission of sensitized acceptor.
Fig. 3. (a) Three dimensional TA signals of the CdTe/CdS QDs alone and (b) CdTe/CdS QDs-Rh101 complexes in water solution at 1atm. (c) TA spectra of QDs alone and (d) CdTe/CdS QDs-Rh101 complexes at 1atm. (e) Kinetics of TA spectra of CdTe/CdS QDs alone and CdTe/CdS QDs-Rh101 complexes. The solid lines correspond to the fittings. (f) Schematic representation of the FRET process and Auger recombination process where energy band diagram indicates the transfer of excitons.
Subsequently, to explore the dependence of pressure on the FRET and Auger recombination lifetime constants, the high-pressure TA spectroscopy of QDs-Rh101 complexes was measured (Fig. S2 in Supplement 1) [45]. The TA kinetic traces of QDs–Rh101 complexes under pressure with global analysis are shown in Fig. S3. The variations in the carrier relaxation process ${\tau _1}$, FRET process ${\tau _{2}}$ and Auger recombination process ${\tau _{3}}$ as a function of pressure are shown in Fig. 4(a-c) (see Table S2 for fitting values). The ratio of Auger recombination process lifetime to FRET process lifetime under high pressure is shown in Fig. 4(d). Figure 4(a) shows that the carrier relaxation lifetime (${\tau _1}$) changes slightly under high pressure. This illustrates that high pressure has little effect on the carrier relaxation process. Importantly, for FRET process, we find that ${\tau _{2}}$ value decreases sharply and finally stabilizes as the pressure increases from 1atm to 0.9Gpa. To explain the reason, we analyzed the factors of affecting FRET rate based on Förster theory. The FRET rate strongly depends on the donor-acceptor distance and is given by Eq. (1) [15,25]:
where ${\tau _D}$ is radiative lifetime of donor and the Förster distance ${R}_0$ is the donor-acceptor distance at which the energy transfer efficiency is 50${\%}$. It can be calculated by the equation [15,25]: where ${\varphi _D}$ is quantum yield of the QD donor, s is the refractive index of the medium, NA is Avogadro’s number, J($\lambda $) is the spectral overlap intergral (see Supplement 1 for calculation details), k2 reflects the relative orientation of the donor and acceptor dipoles, which is a constant (k2 equals to 2/3) [15]. The donor-acceptor separation distance (r) is calculated by using [2]:Fig. 4. (a) Dependence of pressure on the lifetime of the carrier relaxation (${\tau _1}$), (b) FRET process (${\tau _2}$. ), and (c) Auger recombination process (${\tau _3}$). (d) Ratio of Auger recombination process lifetime to FRET process lifetime. (e) Calculated donor-acceptor distance upon compression from 1atm to 0.9Gpa. (f) The number of absorbed acceptor per QDs under pressure from 1atm to 0.9Gpa.
We solve Eq. (4) for $\lambda $ to yield Eq. (5).
where ${B_V}/{B_0}$ is a function of the number of added acceptor. The calculated spectral Overlap J(λ), R0, p for the QD-Rh101 system are summarized in Table 1, and the r and m are shown in Fig. 4(e,f). The m value is the p(n, $\lambda )$ obtained by the Eq. (4) multiplied by the ratio of the acceptor concentration to the donor concentration. The FRET rate [kFRET (${\tau _2}^{ - 1}$)] measured based on TA kinetic fitting. We focus on the analysis of the donor-acceptor distance and the number of absorbed molecules upon compression. As shown in Fig. 4(e,f), the r value gradually decrease. In our system, high pressure can significantly decrease water molecular volume in the liquid, which further induces a reduction in the distance between donor and acceptor. Meanwhile, the m value significantly increases as increasing pressure. This means that pressure induced the reduction of donor-acceptor distance and the increasing of the number absorbed molecules per QDs. As increasing pressure gradually, the FRET time constant is reduced from 130ps at 1atm to 6ps at 0.9 GPa.
Table 1. Summary of the FRET rate (kFRET), spectral overlap J(λ), Förster distance (R0), and possibility (P) of acceptor adsorbed to QDs under several represent pressures.
For Auger recombination process, as shown in Fig. 4(c), the ${\tau _{3}}$ increases significantly as the pressure increase. We speculate that an alloying could form at the core/shell interface in CdTe/CdS QDs. With forming the interface alloy layer, the confinement potential between the core and the shell will be smoothed, which may lead to the observed Auger recombination suppression [23,47,48]. In particular, based on the calculations of Cragg and Efros, the “smooth” interface potential can decrease the Auger recombination rate by more than 3 orders of magnitude [49]. In our research, water acts as a pressure transfer medium upon compression, and a stronger squeezing effect occurs at the core/shell interface. This would lead to enhanced mutual diffusion of Te and S ions and the local strain at the core/shell interface. The local strain causes a greater mismatch between the core and shell crystal lattices, which would offer a driving force for the alloying process [50,51]. As the applied pressure increases, Auger recombination time constant increase from 200ps at 1atm to 425ps at 0.9 GPa. Finally, we observe that the FRET process can occur 70 times faster than Auger recombination process (Fig. 4(d)), indicating high pressure is an efficient tool to simultaneously facilitate the FRET and suppress Auger recombination process.
4. Conclusion
In summary, we have developed a new strategy to efficiently regulate FRET process and Auger recombination process in QDs-molecules system using in situ high-pressure tool. When applying pressure from 1atm to 0.9 GPa to the system, the FRET rate rapidly increases, however, the Auger recombination rate gradually decreases. We ascribe the high rate of FRET to the shortened donor-acceptor distance and the increased the number of adsorbed acceptor. Meanwhile, the highly suppressed Auger recombination is attributed to the formed alloying at the core/shell interface in the QDs upon compression. Intriguingly, the FRET can occur 70 times faster than Auger recombination at 0.9 GPa. The high-rate FRET process, coupled with the low-speed Auger recombination process in QDs-molecules system, suggest great progress in applications including efficient LEDs, solar cells, and optical gain media with lower threshold. Our findings not only develop a new strategy to simultaneously facilitate the FRET and suppress Auger recombination, but also arouse further fundamental research to develop potential applications of QDs-molecules systems.
Funding
National Defense Basic Scientific Research Program of China (2019YFA0307701); National Natural Science Foundation of China (11874180); Young and Middle-aged Scientific and Technological Innovation leaders and Team Projects in Jilin Province (20200301020RQ).
Disclosures
The authors declare no competing financial interests.
Data availability
Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.
Supplemental document
See Supplement 1 for supporting content.
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