1. |
- Abdel-Hafiez, Mahmoud, et al.
(författare)
-
From Insulator to Superconductor : A Series of Pressure-Driven Transitions in Quasi-One-Dimensional TiS3 Nanoribbons
- 2024
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 24:18, s. 5562-5569
-
Tidskriftsartikel (refereegranskat)abstract
- Transition metal trichalcogenides (TMTCs) offer remarkable opportunities for tuning electronic states through modifications in chemical composition, temperature, and pressure. Despite considerable interest in TMTCs, there remain significant knowledge gaps concerning the evolution of their electronic properties under compression. In this study, we employ experimental and theoretical approaches to comprehensively explore the high-pressure behavior of the electronic properties of TiS3, a quasi-one-dimensional (Q1D) semiconductor, across various temperature ranges. Through high-pressure electrical resistance and magnetic measurements at elevated pressures, we uncover a distinctive sequence of phase transitions within TiS3, encompassing a transformation from an insulating state at ambient pressure to the emergence of an incipient superconducting state above 70 GPa. Our findings provide compelling evidence that superconductivity at low temperatures of ∼2.9 K is a fundamental characteristic of TiS3, shedding new light on the intriguing high-pressure electronic properties of TiS3 and underscoring the broader implications of our discoveries for TMTCs in general.
|
|
2. |
- Biswas, Deepnarayan, et al.
(författare)
-
Ultrafast Triggering of Insulator-Metal Transition in Two-Dimensional VSe2
- 2021
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 21:5, s. 1968-1975
-
Tidskriftsartikel (refereegranskat)abstract
- The transition-metal dichalcogenide VSe2 exhibits an increased charge density wave transition temperature and an emerging insulating phase when thinned to a single layer. Here, we investigate the interplay of electronic and lattice degrees of freedom that underpin these phases in single-layer VSe2 using ultrafast pump-probe photoemission spectroscopy. In the insulating state, we observe a light-induced closure of the energy gap, which we disentangle from the ensuing hot carrier dynamics by fitting a model spectral function to the time-dependent photoemission intensity. This procedure leads to an estimated time scale of 480 fs for the closure of the gap, which suggests that the phase transition in single-layer VSe2 is driven by electron-lattice interactions rather than by Mott-like electronic effects. The ultrafast optical switching of these interactions in SL VSe2 demonstrates the potential for controlling phase transitions in 2D materials with light.
|
|
3. |
- Brem, Samuel, 1991, et al.
(författare)
-
Phonon-Assisted Photoluminescence from Indirect Excitons in Monolayers of Transition-Metal Dichalcogenides
- 2020
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 20:4, s. 2849-2856
-
Tidskriftsartikel (refereegranskat)abstract
- The photoluminescence (PL) spectrum of transition-metal dichalcogenides (TMDs) shows a multitude of emission peaks below the bright exciton line, and not all of them have been explained yet. Here, we study the emission traces of phonon-assisted recombinations of indirect excitons. To this end, we develop a microscopic theory describing simultaneous exciton, phonon, and photon interaction and including consistent many-particle dephasing. We explain the drastically different PL below the bright exciton in tungsten- and molybdenum-based materials as the result of different configurations of bright and momentum-dark states. In good agreement with experiments, our calculations predict that WSe2 exhibits clearly visible low-temperature PL signals stemming from the phonon-assisted recombination of momentum-dark K-K′ excitons.
|
|
4. |
- Brem, Samuel, 1991, et al.
(författare)
-
Terahertz Fingerprint of Monolayer Wigner Crystals
- 2022
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 22:3, s. 1311-1315
-
Tidskriftsartikel (refereegranskat)abstract
- The strong Coulomb interaction in monolayer semiconductors represents a unique opportunity for the realization of Wigner crystals without external magnetic fields. In this work, we predict that the formation of monolayer Wigner crystals can be detected by their terahertz response spectrum, which exhibits a characteristic sequence of internal optical transitions. We apply the density matrix formalism to derive the internal quantum structure and the optical conductivity of the Wigner crystal and to microscopically analyze the multipeak shape of the obtained terahertz spectrum. Moreover, we predict a characteristic shift of the peak position as a function of charge density for different atomically thin materials and show how our results can be generalized to an arbitrary two-dimensional system.
|
|
5. |
- Brem, Samuel, 1991, et al.
(författare)
-
Tunable Phases of Moiré Excitons in van der Waals Heterostructures
- 2020
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 20:12, s. 8534-8540
-
Tidskriftsartikel (refereegranskat)abstract
- Stacking monolayers of transition metal dichalcogenides into a heterostructure with a finite twist-angle gives rise to artificial moiré superlattices with a tunable periodicity. As a consequence, excitons experience a periodic potential, which can be exploited to tailor optoelectronic properties of these materials. Whereas recent experimental studies have confirmed twist-angle-dependent optical spectra, the microscopic origin of moiré exciton resonances has not been fully clarified yet. Here, we combine first-principles calculations with the excitonic density matrix formalism to study transitions between different moiré exciton phases and their impact on optical properties of the twisted MoSe2/WSe2 heterostructure. At angles smaller than 2°, we find flat, moiré-trapped states for inter- and intralayer excitons. This moiré exciton phase changes into completely delocalized states at 3°. We predict a linear and quadratic twist-angle dependence of excitonic resonances for the moiré-trapped and delocalized exciton phases, respectively.
|
|
6. |
- Calavalle, Francesco, et al.
(författare)
-
Tailoring Superconductivity in Large-Area Single-Layer NbSe2 via Self-Assembled Molecular Adlayers
- 2021
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 21:1, s. 136-143
-
Tidskriftsartikel (refereegranskat)abstract
- Two-dimensional transition metal dichalcogenides (TMDs) represent an ideal testbench for the search of materials by design, because their optoelectronic properties can be manipulated through surface engineering and molecular functionalization. However, the impact of molecules on intrinsic physical properties of TMDs, such as superconductivity, remains largely unexplored. In this work, the critical temperature (TC) of large-area NbSe2 monolayers is manipulated, employing ultrathin molecular adlayers. Spectroscopic evidence indicates that aligned molecular dipoles within the self-assembled layers act as a fixed gate terminal, collectively generating a macroscopic electrostatic field on NbSe2. This results in an ∼55% increase and a 70% decrease in TC depending on the electric field polarity, which is controlled via molecular selection. The reported functionalization, which improves the air stability of NbSe2, is efficient, practical, up-scalable, and suited to functionalize large-area TMDs. Our results indicate the potential of hybrid 2D materials as a novel platform for tunable superconductivity.
|
|
7. |
- Capobianco, Amedeo, et al.
(författare)
-
Electron Localization and Mobility in Monolayer Fullerene Networks
- 2024
-
Ingår i: Nano Letters. - 1530-6992 .- 1530-6984. ; 24:27, s. 8335-8342
-
Tidskriftsartikel (refereegranskat)abstract
- The novel 2D quasi-hexagonal phase of covalently bonded fullerene molecules (qHP C60), the so-called graphullerene, has displayed far superior electron mobilities, if compared to the parent van der Waals three-dimensional crystal (vdW C60). Herein, we present a comparative study of the electronic properties of vdW and qHP C60 using state-of-the-art electronic-structure calculations and a full quantum-mechanical treatment of electron transfer. We show that both materials entail polaronic localization of electrons with similar binding energies (≈0.1 eV) and, therefore, they share the same charge transport via polaron hopping. In fact, we quantitatively reproduce the sizable increment of the electron mobility measured for qHP C60 and identify its origin in the increased electronic coupling between C60 units.
|
|
8. |
- Carvalho, Pamela C., et al.
(författare)
-
Correlation of Interface Interdiffusion and Skyrmionic Phases
- 2023
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 23:11, s. 4854-4861
-
Tidskriftsartikel (refereegranskat)abstract
- Magnetic skyrmions are prime candidates for the nextgenerationof spintronic devices. Skyrmions and other topological magnetic structuresare known to be stabilized by the Dzyaloshinskii-Moriya interaction(DMI) that occurs when the inversion symmetry is broken in thin films.Here, we show by first-principles calculations and atomistic spindynamics simulations that metastable skyrmionic states can also befound in nominally symmetric multilayered systems. We demonstratethat this is correlated with the large enhancement of the DMI strengthdue to the presence of local defects. In particular, we find thatmetastable skyrmions can occur in Pd/Co/Pd multilayers without externalmagnetic fields and can be stable even near room temperature conditions.Our theoretical findings corroborate with magnetic force microscopyimages and X-ray magnetic circular dichroism measurements and highlightthe possibility of tuning the intensity of DMI by using interdiffusionat thin film interfaces.
|
|
9. |
- Chang, Ribooga, et al.
(författare)
-
Achieving Molecular Sieving of CO2 from CH4 by Controlled Dynamical Movement and Host–Guest Interactions in Ultramicroporous VOFFIVE-1-Ni by Pillar Substitution
- 2024
-
Ingår i: Nano Letters. - 1530-6984 .- 1530-6992. ; 24:25, s. 7616-
-
Tidskriftsartikel (refereegranskat)abstract
- Engineering the building blocks in metal–organic materials is an effective strategy for tuning their dynamical properties and can affect their response to external guest molecules. Tailoring the interaction and diffusion of molecules into these structures is highly important, particularly for applications related to gas separation. Herein, we report a vanadium-based hybrid ultramicroporous material, VOFFIVE-1-Ni, with temperature-dependent dynamical properties and a strong affinity to effectively capture and separate carbon dioxide (CO2) from methane (CH4). VOFFIVE-1-Ni exhibits a CO2 uptake of 12.08 wt% (2.75 mmol g–1), a negligible CH4 uptake at 293 K (0.5 bar), and an excellent CO2-over-CH4 uptake ratio of 2280, far exceeding that of similar materials. The material also exhibits a favorable CO2 enthalpy of adsorption below −50 kJ mol–1, as well as fast CO2 adsorption rates (90% uptake reached within 20 s) that render the hydrolytically stable VOFFIVE-1-Ni a promising sorbent for applications such as biogas upgrading.
|
|
10. |
- Chang, Ribooga, et al.
(författare)
-
Achieving Molecular Sieving of CO2 from CH4 by Controlled Dynamical Movement and Host–Guest Interactions in Ultramicroporous VOFFIVE-1-Ni by Pillar Substitution
- 2024
-
Ingår i: Nano Letters. - 1530-6984 .- 1530-6992. ; 24:25, s. 7616-7622
-
Tidskriftsartikel (refereegranskat)abstract
- Engineering the building blocks in metal–organic materials is an effective strategy for tuning their dynamical properties and can affect their response to external guest molecules. Tailoring the interaction and diffusion of molecules into these structures is highly important, particularly for applications related to gas separation. Herein, we report a vanadium-based hybrid ultramicroporous material, VOFFIVE-1-Ni, with temperature-dependent dynamical properties and a strong affinity to effectively capture and separate carbon dioxide (CO2) from methane (CH4). VOFFIVE-1-Ni exhibits a CO2 uptake of 12.08 wt % (2.75 mmol g–1), a negligible CH4 uptake at 293 K (0.5 bar), and an excellent CO2-over-CH4 uptake ratio of 2280, far exceeding that of similar materials. The material also exhibits a favorable CO2 enthalpy of adsorption below −50 kJ mol–1, as well as fast CO2 adsorption rates (90% uptake reached within 20 s) that render the hydrolytically stable VOFFIVE-1-Ni a promising sorbent for applications such as biogas upgrading.
|
|
11. |
- Chayanun, Lert, et al.
(författare)
-
Direct Three-Dimensional Imaging of an X-ray Nanofocus Using a Single 60 nm Diameter Nanowire Device
- 2020
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 20:11, s. 8326-8331
-
Tidskriftsartikel (refereegranskat)abstract
- Nanoscale X-ray detectors could allow higher resolution in imaging and diffraction experiments than established systems but are difficult to design due to the long absorption length of X-rays. Here, we demonstrate X-ray detection in a single nanowire in which the nanowire axis is parallel to the optical axis. In this geometry, X-ray absorption can occur along the nanowire length, while the spatial resolution is limited by the diameter. We use the device to make a high-resolution 3D image of the 88 nm diameter X-ray nanofocus at the Nanomax beamline, MAX IV synchrotron, by scanning the single pixel device in different planes along the optical axis. The images reveal fine details of the beam that are unattainable with established detectors and show good agreement with ptychography.
|
|
12. |
- Chen, I. Ju, et al.
(författare)
-
Hot-Carrier Extraction in Nanowire-Nanoantenna Photovoltaic Devices
- 2020
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 20:6, s. 4064-4072
-
Tidskriftsartikel (refereegranskat)abstract
- Nanowires bring new possibilities to the field of hot-carrier photovoltaics by providing flexibility in combining materials for band engineering and using nanophotonic effects to control light absorption. Previously, an open-circuit voltage beyond the Shockley-Queisser limit was demonstrated in hot-carrier devices based on InAs-InP-InAs nanowire heterostructures. However, in these first experiments, the location of light absorption, and therefore the precise mechanism of hot-carrier extraction, was uncontrolled. In this Letter, we combine plasmonic nanoantennas with InAs-InP-InAs nanowire devices to enhance light absorption within a subwavelength region near an InP energy barrier that serves as an energy filter. From photon-energy- and irradiance-dependent photocurrent and photovoltage measurements, we find that photocurrent generation is dominated by internal photoemission of nonthermalized hot electrons when the photoexcited electron energy is above the barrier and by photothermionic emission when the energy is below the barrier. We estimate that an internal quantum efficiency up to 0.5-1.2% is achieved. Insights from this study provide guidelines to improve internal quantum efficiencies based on nanowire heterostructures.
|
|
13. |
- Chen, Pan, et al.
(författare)
-
Small Angle Neutron Scattering Shows Nanoscale PMMA Distribution in Transparent Wood Biocomposites
- 2021
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 21:7, s. 2883-2890
-
Tidskriftsartikel (refereegranskat)abstract
- Transparent wood biocomposites based on PMMA combine high optical transmittance with excellent mechanical properties. One hypothesis is that despite poor miscibility the polymer is distributed at the nanoscale inside the cell wall. Small-angle neutron scattering (SANS) experiments are performed to test this hypothesis, using biocomposites based on deuterated PMMA and "contrast-matched" PMMA. The wood cell wall nanostructure soaked in heavy water is quantified in terms of the correlation distance d between the center of elementary cellulose fibrils. For wood/deuterated PMMA, this distance d is very similar as for wood/heavy water (correlation peaks at q approximate to 0.1 angstrom(-1)). The peak disappears when contrast-matched PMMA is used, indeed proving nanoscale polymer distribution in the cell wall. The specific processing method used for transparent wood explains the nanocomposite nature of the wood cell wall and can serve as a nanotechnology for cell wall impregnation of polymers in large wood biocomposite structures.
|
|
14. |
- Chiu, Chun Chien, et al.
(författare)
-
Presence of Delocalized Ti 3d Electrons in Ultrathin Single-Crystal SrTiO3
- 2022
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 22:4, s. 1580-1586
-
Tidskriftsartikel (refereegranskat)abstract
- Strontium titanate (STO), with a wide spectrum of emergent properties such as ferroelectricity and superconductivity, has received significant attention in the community of strongly correlated materials. In the strain-free STO film grown on the SrRuO3 buffer layer, the existing polar nanoregions can facilitate room-temperature ferroelectricity when the STO film thickness approaches 10 nm. Here we show that around this thickness scale, the freestanding STO films without the influence of a substrate show the tetragonal structure at room temperature, contrasting with the cubic structure seen in bulk form. The spectroscopic measurements reveal the modified Ti-O orbital hybridization that causes the Ti ion to deviate from its nominal 4+ valency (3d0 configuration) with excess delocalized 3d electrons. Additionally, the Ti ion in TiO6 octahedron exhibits an off-center displacement. The inherent symmetry lowering in ultrathin freestanding films offers an alternative way to achieve tunable electronic structures that are of paramount importance for future technological applications.
|
|
15. |
- Choi, Junho, et al.
(författare)
-
Fermi Pressure and Coulomb Repulsion Driven Rapid Hot Plasma Expansion in a van der Waals Heterostructure
- 2023
-
Ingår i: Nano Letters. - 1530-6992 .- 1530-6984. ; 23:10, s. 4399-4405
-
Tidskriftsartikel (refereegranskat)abstract
- Transition metal dichalcogenide heterostructures provide a versatile platform to explore electronic and excitonic phases. As the excitation density exceeds the critical Mott density, interlayer excitons are ionized into an electron-hole plasma phase. The transport of the highly non-equilibrium plasma is relevant for high-power optoelectronic devices but has not been carefully investigated previously. Here, we employ spatially resolved pump-probe microscopy to investigate the spatial-temporal dynamics of interlayer excitons and hot-plasma phase in a MoSe2/WSe2 twisted bilayer. At the excitation density of ∼1014 cm-2, well exceeding the Mott density, we find a surprisingly rapid initial expansion of hot plasma to a few microns away from the excitation source within ∼0.2 ps. Microscopic theory reveals that this rapid expansion is mainly driven by Fermi pressure and Coulomb repulsion, while the hot carrier effect has only a minor effect in the plasma phase.
|
|
16. |
- Choi, Seungwoo, et al.
(författare)
-
Kink-Controlled Gold Nanoparticles for Electrochemical Glucose Oxidation
- 2024
-
Ingår i: Nano Letters. - 1530-6984 .- 1530-6992. ; 24:15, s. 4528-4536
-
Tidskriftsartikel (refereegranskat)abstract
- Enzymes in nature efficiently catalyze chiral organic molecules by elaborately tuning the geometrical arrangement of atoms in the active site. However, enantioselective oxidation of organic molecules by heterogeneous electrocatalysts is challenging because of the difficulty in controlling the asymmetric structures of the active sites on the electrodes. Here, we show that the distribution of chiral kink atoms on high-index facets can be precisely manipulated even on single gold nanoparticles; and this enabled stereoselective oxidation of hydroxyl groups on various sugar molecules. We characterized the crystallographic orientation and the density of kink atoms and investigated their specific interactions with the glucose molecule due to the geometrical structure and surface electrostatic potential.
|
|
17. |
- Çlnar, Mustafa Neşet, et al.
(författare)
-
Toward Optimized Charge Transport in Multilayer Reduced Graphene Oxides
- 2022
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 22:6, s. 2202-2208
-
Tidskriftsartikel (refereegranskat)abstract
- In the context of graphene-based composite applications, a complete understanding of charge conduction in multilayer reduced graphene oxides (rGO) is highly desirable. However, these rGO compounds are characterized by multiple and different sources of disorder depending on the chemical method used for their synthesis. Most importantly, the precise role of interlayer interaction in promoting or jeopardizing electronic flow remains unclear. Here, thanks to the development of a multiscale computational approach combining first-principles calculations with large-scale transport simulations, the transport scaling laws in multilayer rGO are unraveled, explaining why diffusion worsens with increasing film thickness. In contrast, contacted films are found to exhibit an opposite trend when the mean free path becomes shorter than the channel length, since conduction becomes predominantly driven by interlayer hopping. These predictions are favorably compared with experimental data and open a road toward the optimization of graphene-based composites with improved electrical conduction.
|
|
18. |
- Debbarma, Rousan, et al.
(författare)
-
Effects of Parity and Symmetry on the Aharonov-Bohm Phase of a Quantum Ring
- 2021
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992.
-
Tidskriftsartikel (refereegranskat)abstract
- We experimentally investigate the properties of one-dimensional quantum rings that form near the surface of nanowire quantum dots. In agreement with theoretical predictions, we observe the appearance of forbidden gaps in the evolution of states in a magnetic field as the symmetry of a quantum ring is reduced. For a twofold symmetry, our experiments confirm that orbital states are grouped pairwise. Here, a π-phase shift can be introduced in the Aharonov-Bohm relation by controlling the relative orbital parity using an electric field. Studying rings with higher symmetry, we note exceptionally large orbital contributions to the effective g-factor (up to 300), which are many times higher than those previously reported. These findings show that the properties of a phase-coherent system can be significantly altered by the nanostructure symmetry and its interplay with wave function parity.
|
|
19. |
- Di, Andi, 1992-, et al.
(författare)
-
Tunable Ordered Nanostructured Phases by Co-assembly of Amphiphilic Polyoxometalates and Pluronic Block Copolymers
- 2023
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 23:5, s. 1645-1651
-
Tidskriftsartikel (refereegranskat)abstract
- The assembly of polyoxometalate (POM) metal–oxygen clusters into ordered nanostructures is attracting a growing interest for catalytic and sensing applications. However, assembly of ordered nanostructured POMs from solution can be impaired by aggregation, and the structural diversity is poorly understood. Here, we present a time-resolved small-angle X-ray scattering (SAXS) study of the co-assembly in aqueous solutions of amphiphilic organo-functionalized Wells-Dawson-type POMs with a Pluronic block copolymer over a wide concentration range in levitating droplets. SAXS analysis revealed the formation and subsequent transformation with increasing concentration of large vesicles, a lamellar phase, a mixture of two cubic phases that evolved into one dominating cubic phase, and eventually a hexagonal phase formed at concentrations above 110 mM. The structural versatility of co-assembled amphiphilic POMs and Pluronic block copolymers was supported by dissipative particle dynamics simulations and cryo-TEM.
|
|
20. |
- Dorsch, Sven, et al.
(författare)
-
Heat Driven Transport in Serial Double Quantum Dot Devices
- 2021
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 21:2, s. 988-994
-
Tidskriftsartikel (refereegranskat)abstract
- Studies of thermally induced transport in nanostructures provide access to an exciting regime where fluctuations are relevant, enabling the investigation of fundamental thermodynamic concepts and the realization of thermal energy harvesters. We study a serial double quantum dot formed in an InAs/InP nanowire coupled to two electron reservoirs. By means of a specially designed local metallic joule-heater, the temperature of the phonon bath in the vicinity of the double quantum dot can be enhanced. This results in phonon-assisted transport, enabling the conversion of local heat into electrical power in a nanosized heat engine. Simultaneously, the electron temperatures of the reservoirs are affected, resulting in conventional thermoelectric transport. By detailed modeling and experimentally tuning the interdot coupling, we disentangle both effects. Furthermore, we show that phonon-assisted transport is sensitive to excited states. Our findings demonstrate the versatility of our design to study fluctuations and fundamental nanothermodynamics.
|
|
21. |
- Eremchev, Ivan Yu, et al.
(författare)
-
Detection of Single Charge Trapping Defects in Semiconductor Particles by Evaluating Photon Antibunching in Delayed Photoluminescence
- 2023
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992.
-
Tidskriftsartikel (refereegranskat)abstract
- Time-resolved analysis of photon cross-correlation function g(2)(τ) is applied to photoluminescence (PL) of individual submicrometer size MAPbI3 perovskite crystals. Surprisingly, an antibunching effect in the long-living tail of PL is observed, while the prompt PL obeys the photon statistics typical for a classical emitter. We propose that antibunched photons from the PL decay tail originate from radiative recombination of detrapped charge carriers which were initially captured by a very limited number (down to one) of shallow defect states. The concentration of these trapping sites is estimated to be in the range 1013-1016 cm-3. In principle, photon correlations can be also caused by highly nonlinear Auger recombination processes; however, in our case it requires unrealistically large Auger recombination coefficients. The potential of the time-resolved g(2)(0) for unambiguous identification of charge rerecombination processes in semiconductors considering the actual number of charge carries and defects states per particle is demonstrated.
|
|
22. |
- Fang, Cheng, et al.
(författare)
-
An Autoclavable and Transparent Thermal Cutter for Reliably Sealing Wet Nanofibrous Membranes
- 2024
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 24:28, s. 8709-8716
-
Tidskriftsartikel (refereegranskat)abstract
- Sealing wet porous membranes is a major challenge when fabricating cell encapsulation devices. Herein, we report the development of an Autoclavable Transparent Thermal Cutter (ATTC) for reliably sealing wet nanofibrous membranes. Notably, the ATTC is autoclavable and transparent, thus enabling in situ visualization of the sealing process in a sterile environment and ensuring an appropriate seal. In addition, the ATTC could generate smooth, arbitrary-shaped sealing ends with excellent mechanical properties when sealing PA6, PVDF, and TPU nanofibrous tubes and PP microporous membranes. Importantly, the ATTC could reliably seal wet nanofibrous tubes, which can shoulder a burst pressure up to 313.2 +/- 19.3 kPa without bursting at the sealing ends. Furthermore, the ATTC sealing process is highly compatible with the fabrication of cell encapsulation devices, as verified by viability, proliferation, cell escape, and cell function tests. We believe that the ATTC could be used to reliably seal cell encapsulation devices with minimal side effects.
|
|
23. |
- Fitzgerald, Jamie, 1992, et al.
(författare)
-
Twist Angle Tuning of Moiré Exciton Polaritons in van der Waals Heterostructures
- 2022
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 22:11, s. 4468-4474
-
Tidskriftsartikel (refereegranskat)abstract
- Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist angle. We find that these new hybrid light-exciton states become delocalized relative to the constituent excitons due to the mixing with light and higher-energy excitons. The system can be interpreted as a natural quantum metamaterial with a periodicity that can be engineered via the twist angle. Our study presents a significant advance in microscopic understanding and control of moiré exciton polaritons in twisted atomically thin semiconductors.
|
|
24. |
- Fojt, Jakub, 1996, et al.
(författare)
-
Hot-Carrier Transfer across a Nanoparticle-Molecule Junction: The Importance of Orbital Hybridization and Level Alignment
- 2022
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6992 .- 1530-6984. ; 22:21, s. 8786-8792
-
Tidskriftsartikel (refereegranskat)abstract
- While direct hot-carrier transfer can increase photocatalytic activity, it is difficult to discern experimentally and competes with several other mechanisms. To shed light on these aspects, here, we model from first-principles hot-carrier generation across the interface between plasmonic nanoparticles and a CO molecule. The hot-electron transfer probability depends nonmonotonically on the nanoparticle-molecule distance and can be effective at long distances, even before a strong chemical bond can form; hot-hole transfer on the other hand is limited to shorter distances. These observations can be explained by the energetic alignment between molecular and nanoparticle states as well as the excitation frequency. The hybridization of the molecular orbitals is the key predictor for hot-carrier transfer in these systems, emphasizing the necessity of ground state hybridization for accurate predictions. Finally, we show a nontrivial dependence of the hot-carrier distribution on the excitation energy, which could be exploited when optimizing photocatalytic systems.
|
|
25. |
- Fransson, Jonas, 1970-
(författare)
-
Charge Redistribution and Spin Polarization Driven by Correlation Induced Electron Exchange in Chiral Molecules
- 2021
-
Ingår i: Nano Letters. - : American Chemical Society (ACS). - 1530-6984 .- 1530-6992. ; 21:7, s. 3026-3032
-
Tidskriftsartikel (refereegranskat)abstract
- Chiral induced spin selectivity is a phenomenon that has been attributed to chirality, spin-orbit interactions, and nonequilibrium conditions, while the role of electron exchange and correlations have been investigated only marginally until very recently. However, as recent experiments show that chiral molecules acquire a finite spin-polarization merely by being in contact with a metallic surface, these results suggest that electron correlations play a more crucial role for the emergence of the phenomenon than previously thought. Here, it is demonstrated that molecular vibrations give rise to molecular charge redistribution and accompany spin-polarization when coupling a chiral molecule to a nonmagnetic metal. The presented theory opens up new routes to construct a comprehensive picture of enantiomer separation.
|
|