Boldt, Klaus

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Control of Hot Carrier Relaxation in CsPbBr3 Nanocrystals Using Damping Ligands

2022, Zeng, Peng, Ren, Xinjian, Wei, Linfeng, Zhao, Haifeng, Liu, Xiaochun, Zhang, Xinyang, Xu, Yanmin, Yan, Lihe, Boldt, Klaus, Smith, Trevor A.

In photon-conversion processes, rapid cooling of photo-induced hot carriers is a dominant energy loss channel. We herein report a 3-fold reduced hot carrier cooling rate in CsPbBr 3 nanocrystals capped with a cross-linked polysiloxane shell in comparison to single alkyl-chain oleylamine ligands. Relaxation of hot charge carriers depends on the carrier-phonon coupling (CPC) process as an important channel to dissipate energies in nanostructured perovskite materials. The CPC strengths in the two samples were measured through cryogenic photoluminescence spectroscopic measurements. The effect of organic ligands on the CPC in CsPbBr 3 nanocrystals is elucidated based on a damped oscillation model. This supplements the conventional polaron-based CPC model, by involving a damping effect on the CPC from the resistance of the ligands against nanocrystal lattice vibrations. The model also accounts for the observed linear temperature-dependence of the CPC strength. Our work enables predictions about the effect of the ligands on the performance of perovskite nanocrystals in future applications.

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Electronic Structure Engineering in ZnSe/CdS Type-II Nanoparticles by Interface Alloying

2014-06-19, Boldt, Klaus, Schwarz, Kyra N., Kirkwood, Nicholas, Smith, Trevor A., Mulvaney, Paul

We report the synthesis and characterization of type-II ZnSe/CdS semiconductor nanocrystals that exhibit strong charge separation, high photoluminescence quantum yields, low optical gain thresholds, and alloyed core–shell interfaces. Shell growth rates and the degree of alloying both depend strongly on the shelling temperature. The core–shell NCs exhibit band edge PL with emission wavelengths spanning the blue to orange region of the electromagnetic spectrum (380–562 nm). Fluorescence quantum yields up to 75% can be obtained by deposition of an additional ZnS layer. Transient absorption spectroscopy reveals that the population of the first two exciton states (1Se–1Sh, 1Se–2Sh) in the type-II structures can be controlled by alloying. Increased alloying leads to a greater population of the 2S hole state exciton.

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Switchable dissociation of excitons bound at strained CdTe/CdS interfaces

2018-12-06, Enders, Florian, Budweg, Arne, Zeng, Peng, Lauth, Jannika, Smith, Trevor A., Brida, Daniele, Boldt, Klaus

Charge carrier dynamics of semiconductor nano-heterostructures are determined by band alignment and lattice mismatch of the adjacent materials. However, quantum efficiencies for the separation of excited charge carriers at such an interface are hard to predict and cannot yet be easily controlled. In this work we examine nanorods with a severely strained, axial CdTe/CdS interface using femtosecond transient absorption spectroscopy. We show that charge separation is mitigated by equal contributions of valence band distortion and formation of coulomb pairs across the interface. Left undisturbed such localised excitons relax rapidly via non-radiative recombination channels. By adding a competitive hole acceptor that disrupts the coulomb interaction we overcome the synergetic co-localisation of the carriers and realise charge separation. The thus created long-lived state can be exploited for a broad range of applications such as photocatalysis, water splitting, and switchable nanodevices.

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Shell effects on hole-coupled electron transfer dynamics from CdSe/CdS quantum dots to methyl viologen

2016, Zeng, Peng, Kirkwood, Nicholas, Mulvaney, Paul, Boldt, Klaus, Smith, Trevor A.

Electron transfer (ET) dynamics from the 1Se electron state in quasi-type II CdSe/CdS core/shell quantum dots (QDs) to adsorbed methyl viologen (MV(2+)) were measured using femtosecond transient absorption spectroscopy. The intrinsic ET rate kET was determined from the measured average number of ET-active MV(2+) per QD, which permits reliable comparisons of variant shell thickness and different hole states. The 1Se electron was extracted efficiently from the CdSe core, even for CdS shells up to 20 Å thick. The ET rate decayed exponentially from 10(10) to 10(9) s(-1) for increasing CdS shell thicknesses with an attenuation factor β≈ 0.13 Å(-1). We observed that compared to the ground state exciton 1Se1S3/2 the electron coupled to the 2S3/2 hot hole state exhibited slower ET rates for thin CdS shells. We attribute this behaviour to an Auger-assisted ET process (AAET), which depends on electron-hole coupling controlled by the CdS shell thickness.