A phase transition material, VO 2 , with a semiconductor-to-metal transition (SMT) near 341 K (68 °C) has attracted significant research interest because of drastic changes in its electrical resistivity and optical dielectric properties. To address its application needs at specific temperatures, tunable SMT temperatures are highly desired. In this work, effective transition temperature ( T c ) tuning of VO 2 has been demonstrated via a novel Pt : VO 2 nanocomposite design, i.e. , uniform Pt nanoparticles (NPs) embedded in the VO 2 matrix. Interestingly, a bidirectional tuning has been achieved, i.e. , the transition temperature can be systematically tuned to as low as 329.16 K or as high as 360.74 K, with the average diameter of Pt NPs increasing from 1.56 to 4.26 nm. Optical properties, including transmittance ( T %) and dielectric permittivity ( ε ′) were all effectively tuned accordingly. All Pt : VO 2 nanocomposite thin films maintain reasonable SMT properties, i.e. sharp phase transition and narrow width of thermal hysteresis. The bidirectional T c tuning is attributed to two factors: the reconstruction of the band structure at the Pt : VO 2 interface and the change of the Pt : VO 2 phase boundary density. This demonstration sheds light on phasemore »
Temperature dependence of photophysical properties of a dinuclear C^N-cyclometalated Pt( ii ) complex with an intimate Pt–Pt contact. Zero-field splitting and sub-state decay rates of the lowest triplet
The temperature dependence (1.7 K < T < 100 K) of emission decay is reported for the first time for a type of di-nuclear Pt complex featuring a metal–metal-to-ligand charge transfer (MMLCT) lowest energy transition that arises from a strong Pt–Pt interaction. The effect of local variation of the host/guest cage in a polymer matrix upon the phosphorescence decay time constants is characterized by the Kohlrausch–Williams–Watts function. The temperature dependence of the average decay time constants is fit by a Boltzmann-type expression to obtain the average zero-field splittings and individual sublevel decay rates of the photoluminescent triplet excited state.
- Award ID(s):
- 1665033
- Publication Date:
- NSF-PAR ID:
- 10103955
- Journal Name:
- Physical Chemistry Chemical Physics
- Volume:
- 20
- Issue:
- 38
- Page Range or eLocation-ID:
- 25096 to 25104
- ISSN:
- 1463-9076
- Sponsoring Org:
- National Science Foundation
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Ultrafast excited state processes of transition metal complexes (TMCs) are governed by complicated interplays between electronic and nuclear dynamics, which demand a detailed understanding to achieve optimal functionalities of photoactive TMC-based materials for many applications. In this work, we investigated a cyclometalated platinum( ii ) dimer known to undergo a Pt–Pt bond contraction in the metal–metal-to-ligand-charge-transfer (MMLCT) excited state using femtosecond broadband transient absorption (fs-BBTA) spectroscopy in combination with geometry optimization and normal mode calculations. Using a sub-20 fs pump and broadband probe pulses in fs-BBTA spectroscopy, we were able to correlate the coherent vibrational wavepacket (CVWP) evolution with the stimulated emission (SE) dynamics of the 1 MMLCT state. The results demonstrated that the 145 cm −1 CVWP motions with the damping times of ∼0.9 ps and ∼2 ps originate from coherent Pt–Pt stretching vibrations in the singlet and triplet MMLCT states, respectively. On the basis of excited state potential energy surface calculations in our previous work, we rationalized that the CVWP transfer from the Franck–Condon (FC) state to the 3 MMLCT state was mediated by a triplet ligand-centered ( 3 LC) intermediate state through two step intersystem crossing (ISC) on a time scale shorter than a period of themore »
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Temperature-dependent continuous-excitation and time-resolved photoluminescence are studied to probe carrier localization and recombination in nearly strain-balanced m-plane In0.09Ga0.91N/Al0.19Ga0.81N multi-quantum wells grown by plasma-assisted molecular-beam epitaxy. An average localization depth of 21 meV is estimated for the undoped sample. This depth is much smaller than the reported values in polar structures and m-plane InGaN quantum wells. As part of this study, temperature and magnetic field dependence of time-resolved photoluminescence is performed. At 2 K, an initial fast decay time of 0.3 ns is measured for both undoped and doped structures. The undoped sample also exhibits a slow decay component with a time scale of 2.2 ns. The existence of two relaxation paths in the undoped structure can be attributed to different localization centers. The fast relaxation decays are relatively insensitive to external magnetic fields, while the slower relaxation time constant decreases significantly with increasing magnetic fields. The fast decay time scale in the undoped sample is likely due to indium fluctuations in the quantum well. The slow decay time may be related to carrier localization in the barriers. The addition of doping leads to a single fast decay time likely due to stronger exciton localization in the InGaN quantum wells.
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Publisher's Version of Record
- https://doi.org/10.1039/c8cp05213a
