251. Advanced Materials for Energy-Water Systems: The Central Role of Water/Solid Interfaces in Adsorption, Reactivity, and Transport
Edward Barry, Raelyn Burns, Wei Chen, Guilhem X De Hoe, Joan Manuel Montes De Oca, Juan J de Pablo, James Dombrowski, Jeffrey W Elam, Alanna M Felts, Giulia Galli, John Hack, Qiming He, Xiang He, Eli Hoenig, Aysenur Iscen, Benjamin Kash, Harold H Kung, Nicholas HC Lewis, Chong Liu, Xinyou Ma, Anil Mane, Alex BF Martinson, Karen L Mulfort, Julia Murphy, Kristian Mølhave, Paul Nealey, Yijun Qiao, Vepa Rozyyev, George C Schatz, Steven J Sibener, Dmitri Talapin, David M Tiede, Matthew V Tirrell, Andrei Tokmakoff, Gregory A Voth, Zhongyang Wang, Zifan Ye, Murat Yesibolati, Nestor J Zaluzec, Seth B Darling. Chem. Rev. 2021.
The structure, chemistry, and charge of interfaces between materials and aqueous fluids play a central role in determining properties and performance of numerous water systems. Sensors, membranes, sorbents, and heterogeneous catalysts almost uniformly rely on specific interactions between their surfaces and components dissolved or suspended in the water—and often the water molecules themselves—to detect and mitigate contaminants. Deleterious processes in these systems such as fouling, scaling (inorganic deposits), and corrosion are also governed by interfacial phenomena. Despite the importance of these interfaces, much remains to be learned about their multiscale interactions. Developing a deeper understanding of the molecular- and mesoscale phenomena at water/solid interfaces will be essential to driving innovation to address grand challenges in supplying sufficient fit-for-purpose water in the future. In this Review, we examine the current state of knowledge surrounding adsorption, reactivity, and transport in several key classes of water/solid interfaces, drawing on a synergistic combination of theory, simulation, and experiments, and provide an outlook for prioritizing strategic research directions.
Quasi-two-dimensional semiconductor nanoplatelets (NPLs) are intriguing systems for studying the influence of Auger recombination processes on the multiexciton emission efficiencies in the weak in-plane confinement regime. We investigate CdSe/CdS core/shell NPLs using cryogenic temperature single particle spectroscopy and observe bright biexciton emission at high excitation powers. The average binding energy of the biexcitons is determined to be 16.5 meV. The observed switching between the biexciton and trion states indicates charging-decharging dynamics of the NPLs mediated by the Auger ionization process. These findings are highly relevant for harvesting efficient biexciton emission for energy, lighting, and quantum applications.
249. Nanoscale Disorder Generates Subdiffusive Heat Transport in Self-Assembled Nanocrystal Films
James K Utterback, Aditya Sood, Igor Coropceanu, Burak Guzelturk, Dmitri V Talapin, Aaron M Lindenberg, Naomi S Ginsberg. Nano Lett. 2021, 21, 8, 3540–3547.
Investigating the impact of nanoscale heterogeneity on heat transport requires a spatiotemporal probe of temperature on the length and time scales intrinsic to heat navigating nanoscale defects. Here, we use stroboscopic optical scattering microscopy to visualize nanoscale heat transport in disordered films of gold nanocrystals. We find that heat transport appears subdiffusive at the nanoscale. Finite element simulations show that tortuosity of the heat flow underlies the subdiffusive transport, owing to a distribution of nonconductive voids. Thus, while heat travels diffusively through contiguous regions of the film, the tortuosity causes heat to navigate circuitous pathways that make the observed mean-squared expansion of an initially localized temperature distribution appear subdiffusive on length scales comparable to the voids. Our approach should be broadly applicable to uncover the impact of both designed and unintended heterogeneities in a wide range of materials and devices that can affect more commonly used spatially averaged thermal transport measurements.
248. Room temperature single-photon superfluorescence from a single epitaxial cuboid nano-heterostructure
John P Philbin, Joseph Kelly, Lintao Peng, Igor Coropceanu, Abhijit Hazarika, Dmitri V Talapin, Eran Rabani, Xuedan Ma, Prineha Narang. arXiv. 2021.
Single-photon superradiance can emerge when a collection of identical emitters are spatially separated by distances much less than the wavelength of the light they emit, and is characterized by the formation of a superradiant state that spontaneously emits light with a rate that scales linearly with the number of emitters. This collective phenomena has only been demonstrated in a few nanomaterial systems, all requiring temperatures below 10K. Here, we rationally design a single colloidal nanomaterial that hosts multiple (nearly) identical emitters that are impervious to the fluctuations which typically inhibit room temperature superradiance in other systems such as molecular aggregates. Specifically, by combining molecular dynamics, atomistic electronic structure calculations, and model Hamiltonian methods, we show that the faces of a heterostructure nanocuboid mimic individual quasi-2D nanoplatelets and can serve as the robust emitters required to realize superradiant phenomena at room temperature. Leveraging layer-by-layer colloidal growth techniques to synthesize a nanocuboid, we demonstrate single-photon superfluorescence via single-particle time-resolved photoluminescence measurements at room temperature. This robust observation of both superradiant and subradiant states in single nanocuboids opens the door to ultrafast single-photon emitters and provides an avenue to entangled multi-photon states via superradiant cascades.
247. Dynamic lattice distortions driven by surface trapping in semiconductor nanocrystals
Burak Guzelturk, Benjamin L Cotts, Dipti Jasrasaria, John P Philbin, David A Hanifi, Brent A Koscher, Arunima D Balan, Ethan Curling, Marc Zajac, Suji Park, Nuri Yazdani, Clara Nyby, Vladislav Kamysbayev, Stefan Fischer, Zach Nett, Xiaozhe Shen, Michael E Kozina, Ming-Fu Lin, Alexander H Reid, Stephen P Weathersby, Richard D Schaller, Vanessa Wood, Xijie Wang, Jennifer A Dionne, Dmitri V Talapin, A Paul Alivisatos, Alberto Salleo, Eran Rabani, Aaron M Lindenberg. Nat. Com. 2021, 12, 1.
Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in such materials are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in colloidal semiconductor nanocrystals. Investigation of the excitation energy dependence in a core/shell system shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nanocrystal surfaces on few picosecond timescales associated with the localization of trapped holes. On the other hand, carriers created by a photon energy close to the bandgap of the core in the same system result in transient lattice heating that occurs on a much longer 200 picosecond timescale, dominated by an Auger heating mechanism. Elucidation of the structural deformations associated with the surface trapping of hot holes provides atomic-scale insights into the mechanisms deteriorating optoelectronic performance and a pathway towards minimizing these losses in nanocrystal devices.
246. Direct Optical Lithography of Colloidal Metal Oxide Nanomaterials for Diffractive Optical Elements with 2π Phase Control
Jia-Ahn Pan, Zichao Rong, Yuanyuan Wang, Himchan Cho, Igor Coropceanu, Haoqi Wu, and Dmitri V. Talapin. J. Am. Chem. Soc. 2021, 143, 5, 2372–2383.
Spatially patterned dielectric materials are ubiquitous in electronic, photonic, and optoelectronic devices. These patterns are typically made by subtractive or additive approaches utilizing vapor-phase reagents. On the other hand, recent advances in solution-phase synthesis of oxide nanomaterials have unlocked a materials library with greater compositional, microstructural, and interfacial tunability. However, methods to pattern and integrate these nanomaterials in real-world devices are less established. In this work, we directly optically pattern oxide nanoparticles (NPs) by mixing them with photosensitive diazo-2-naphthol-4-sulfonic acid and irradiating with widely available 405 nm light. We demonstrate the direct optical lithography of ZrO2, TiO2, HfO2, and ITO NPs and investigate the chemical and physical changes responsible for this photoinduced decrease in solubility. For example, micron-thick layers of amorphous ZrO2 NPs were patterned with micron resolution and shown to allow 2pi phase control of visible light. We also show multilayer patterning and use it to fabricate features with different thicknesses and distinct structural colors. Upon annealing at 400 C, the deposited structures have excellent optical transparency across a wide wavelength range (0.3 – 10 um), a high refractive index (n = 1.84 at 633 nm) and are optically smooth. We then fabricate diffractive optical elements, such as binary phase diffraction gratings, that show efficient diffractive behavior and good thermal stability. Different oxide NPs can also be mixed prior to patterning, providing a high level of material tunability. This work demonstrates a general patterning approach that harnesses the processability and diversity of colloidal oxide nanomaterials for use in photonic applications.
245. Stoichiometry of the Core Determines the Electronic Structure of Core–Shell III–V/II–VI Nanoparticles
Mariami Rusishvili, Stefan Wippermann, Dmitri V. Talapin, and Giulia Galli. Chem. Mater. 2020, 32, 9798-9804.
244. Functional materials and devices by self-assembly
Dmitri V. Talapin, Michael Engel, and Paul V. Braun. MRS Bull. 2020, 45, 799.
243. Direct Optical Patterning of Quantum Dot Light‐Emitting Diodes via In Situ Ligand Exchange
Himchan Cho, Jia‐Ahn Pan, Haoqi Wu, Xinzheng Lan, Igor Coropceanu, Yuanyuan Wang, Wooje Cho, Ethan A. Hill, John S. Anderson, and Dmitri V. Talapin. Adv. Mater. 2020, 32, 2003805.
242. Area and thickness dependence of Auger recombination in nanoplatelets
John P. Philbin, Alexandra Brumberg, Benjamin T. Diroll, Wooje Cho, Dmitri V. Talapin, Richard D. Schaller, and Eran Rabani. J. Chem. Phys. 2020, 153, 054104.
241. Covalent surface modifications and superconductivity of two-dimensional metal carbide MXenes
Vladislav Kamysbayev, Alexander S. Filatov, Huicheng Hu, Xue Rui, Francisco Lagunas, Di Wang, Robert F. Klie, and Dmitri V. Talapin. Science 2020, 369, 979.
240. sasPDF: pair distribution function analysis of nanoparticle assemblies from small-angle scattering data
Chia-Hao Liu, Eric M. Janke, Ruipen Li, Pavol Juhás, Oleg Gang, Dmitri V. Talapin, and Simon J. L. Billinge. J. Appl. Cryst. 2020, 53, 699.
239. Bright trion emission from semiconductor nanoplatelets
Lintao Peng, Matthew Otten, Abhijit Hazarika, Igor Coropceanu, Moritz Cygorek, Gary P. Wiederrecht, Pawel Hawrylak, Dmitri V. Talapin, and Xuedan Ma. Phys. Rev. Materials 2020, 4, 056006.
238. Heat-driven acoustic phonons in lamellar nanoplatelet assemblies
Benjamin T. Diroll, Vladislav Kamysbayev, Igor Coropceanu, Dmitri V. Talapin, and Richard D. Schaller. Nanoscale 2020, 12, 9661.
237. Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy
Burak Guzelturk, James K. Utterback, Igor Coropceanu, Vladislav Kamysbayev, Eric M. Janke, Marc Zajac, Nuri Yazdani, Benjamin L. Cotts, Suji Park, Aditya Sood, Ming-Fu Lin, Alexander H. Reid, Michael E. Kozina, Xiaozhe Shen, Stephen P. Weathersby, Vanessa Wood, Alberto Salleo, Xijie Wang, Dmitri V. Talapin, Naomi S. Ginsberg, and Aaron M. Lindenberg. ACS Nano 2020, 14, 4792.
236. Quantized Reaction Pathways for Solution Synthesis of Colloidal ZnSe Nanostructures: A Connection between Clusters, Nanowires, and Two-Dimensional Nanoplatelets
P. D. Cunningham, Igor Coropceanu, K. Mulloy, W. Cho, D. V. Talapin. ACS Nano 2020, 14, 3847.
235. Quantum dot solids showing state-resolved band-like transport
X. Lan, M. Chen, M. H. Hudson, V. Kamysbayev, Y. Wang, P. Guyot-Sionnest, and D. V. Talapin. Nature Mater. 2020, 19, 323.
234. Hot-Carrier Relaxation in CdSe/CdS Core/Shell Nanoplatelets
M. Pelton, Y, Wang, I. Fedin, D. V. Talapin, S. K. O’Leary. J. Phys. Chem. C 2020, 124, 1020.
233. Titanium Nitride Modified Photoluminescence from Single Semiconductor Nanoplatelets
L. Peng, X. Wang, I. Coropceanu, A. B. Martinson, H. Wang, D. V. Talapin, and X. Ma. Adv. Funct. Mater. 2020, 30, 1904179.
232. Direct Wavelength-Selective Optical and Electron-Beam Lithography of Functional Inorganic Nanomaterials
Y. Wang, J.-A. Pan, H. Wu, and D. V. Talapin. ACS Nano 2019, 13, 13917.
231. Colloidal Gelation in Liquid Metals Enables Functional Nanocomposites of 2D Metal Carbides (MXenes) and Lightweight Metals
V. Kamysbayev, N. M. James, A. S. Filatov, V. Srivastava, B. Anasori, H. M. Jaeger, Y. Gogotsi, and D. V. Talapin. ACS Nano 2019, 13, 12415.
230. Polarized near-infrared intersubband absorptions in CdSe colloidal quantum wells
B. T. Diroll, M. Chen, I. Coropceanu, K. R. Williams, D. V. Talapin, P. Guyot-Sionnest, and R. D. Schaller. Nat. Commun. 2019, 10, 4511.
229. High Carrier Mobility in HgTe Quantum Dot Solids Improves Mid-IR Photodetectors
M. Chen, X. Lan, X. Tang, Y. Wang, M. H. Hudson, D. V. Talapin, and P. Guyot-Sionnest. ACS Photonics 2019, 6, 2358.
228. Colloidal Atomic Layer Deposition with Stationary Reactant Phases Enables Precise Synthesis of “Digital” II-VI Nano-heterostructures with Exquisite Control of Confinement and Strain
A. Hazarika, I. Fedin, L. Hong, J. Guo, V. Srivastava, W. Cho, I. Coropceanu, J. C. Portner, B. T. Diroll, J. P. Philbin, E. Rabani, R. F. Klie, and D. V. Talapin. J. Am. Chem. Soc. 2019, 141, 13487.
227. Uniaxial transition dipole moments in semiconductor quantum rings caused by broken rotational symmetry
N. F. Hartmann, M. Otten, I. Fedin, D. V. Talapin, M. Cygorek, P. Hawrylak, M. Korkusinski, S. Gray, A. Hartschuh, and X. Ma. Nat. Commun. 2019, 10, 3253.
226. Binary Assembly of PbS and Au Nanocrystals: Patchy PbS Surface Ligand Coverage Stabilizes the CuAu Superlattice
M. Boles and D. V. Talapin. ACS Nano 2019, 13, 5375.
225. Nanocrystals in Molten Salts and Ionic Liquids: Experimental Observation of Ionic Correlations Extending beyond the Debye Length
V. Kamysbayev, V. Srivastava, N. B. Ludwig, O. J. Borkiewicz, H. Zhang, J. Ilavsky, B. Lee, K. W. Chapman, S. Vaikuntanathan, D. V. Talapin. ACS Nano 2019, 13, 5760.
224. Systematic Mapping of Binary Nanocrystal Superlattices: The Role of Topology in Phase Selection
I. Coropceanu, M. A. Boles, D. V. Talapin. J. Am. Chem. Soc. 2019, 141, 5728.
223. Describing screening in dense ionic liquids with a charge-frustrated Ising model
N. B. Ludwig, K. Dasbiswas, D. V. Talapin, S. Vaikuntanathan. J. Chem. Phys. 2018, 149, 164505.
222. Origin of Broad Emission Spectra in InP Quantum Dots: Contributions from Structural and Electronic Disorder
E. M. Janke, N. E. Williams, C. She, D. Zherebetskyy, M. Hudson, L. Wang, D. J. Gosztola, R. D. Schaller, B. Lee, C. Sun, G. S. Engel, D. V. Talapin. J. Am. Chem. Soc. 2018, 140, 15791.
221. Direct Synthesis of Six-Monolayer (1.9 nm) Thick Zinc-Blende CdSe Nanoplatelets Emitting at 585 nm
W. Cho, S. Kim, I. Coropceanu, V. Srivastava, B. T. Diroll, A. Hazarika, I. Fedin, R. D. Schaller, G. Galli, D. V. Talapin. Chem. Mater. 2018, 30, 6957.
220. Semiconductor Nanoplatelet Excimers
B. T. Diroll, W. Cho, I. Coropceanu, S. Harvey, A. Brumberg, N. Holtgrewe, S. A. Crooker, M. R. Wasielewski, V. B. Prakapenka, D. V. Talapin, R. D. Schaller. Nano Lett. 2018, 18, 6948.
219. Colloidal Chemistry in Molten Salts: Synthesis of Luminescent In1–xGaxP and In1–xGaxAs Quantum Dots
V. Srivastava, V. Kamysbayev, L. Hong, E. Dunietz, R. F. Klie, D. V. Talapin. J. Am. Chem. Soc. 2018, 140, 12144.
218. Conduction Band Fine Structure in Colloidal HgTe Quantum Dots
M. H. Hudson, M. Chen, V. Kamysbayev, E. M. Janke, X. Lan, G. Allan, C. Delerue, B. Lee, P. Guyot-Sionnest, D. V. Talapin. ACS Nano 2018, 12, 9397.
217. Anisotropic photoluminescence from isotropic optical transition dipoles in semiconductor nanoplatelets
X. Ma, B. T. Diroll, W. Cho, I. Fedin, R. D. Schaller, D. V. Talapin, and G. P. Wiederrecht. Nano Lett. 2018, 18, 4647.
216. Surface chemistry and buried interfaces in all-inorganic nanocrystalline solids
E. Scalise, V. Srivastava, E. M. Janke, D. Talapin, G. Galli, and S. Wippermann. Nature Nanotech. 2018, 33, 841.
215. Monodisperse InAs Quantum Dots from Aminoarsine Precursors: Understanding the Role of Reducing Agent
V. Srivastava, E. Dunietz, V. Kamysbayev, J. S. Anderson, and D. V. Talapin. Chem. Mater. 2018, 30, 3623.
214. Elevated Temperature Photophysical Properties and Morphological Stability of CdSe and CdSe/CdS Nanoplatelets
C. E. Rowland, I. Fedin, B. T. Diroll, Y. Liu, D. V. Talapin, and R. D. Schaller. J. Phys. Chem. Lett. 2018, 9, 286.
213. Nonmonotonic Dependence of Auger Recombination Rate on Shell Thickness for CdSe/CdS Core/Shell Nanoplatelets
M. Pelton, J. J. Andrews, I. Fedin, D. V. Talapin, H. Lengd S. K. O’Leary. Nano Lett. 2017, 17, 6900.
212. Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets
X. Ma, B. T. Diroll, W. Cho, I. Fedin, R. D. Schaller, D. V. Talapin, S. K. Gray, G. P. Wiederrecht, and D. J. Gosztola. ACS Nano 2017, 11, 9119.
211. Direct optical lithography of functional inorganic nanomaterials
Y. Wang, I. Fedin, H. Zhang, and D. V. Talapin. Science 2017, 357, 385.
Perspective: M. Striccoli. Photolithography based on nanocrystals. Science 2017, 357, 353.
210. A room temperature continuous-wave nanolaser using colloidal quantum wells
Z. Yang, M. Pelton, I. Fedin, D. V. Talapin, and E. Waks. Nat. Commun. 2017, 8, 143.
209. Soluble Lead and Bismuth Chalcogenidometallates: Versatile Solders for Thermoelectric Materials
H. Zhang, J. S. Son, D. S. Dolzhnikov, A. S. Filatov, A. Hazarika, Y. Wang, M. H. Hudson, C.-J. Sun, S. Chattopadhyay, and D. V. Talapin. Chem. Mater. 2017, 29, 6396.
208. Orbitals, Occupation Numbers, and Band Structure of Short One-Dimensional Cadmium Telluride Polymers
A. J. S. Valentine, D. V. Talapin, and D. A. Mazziotti. J. Phys. Chem. A 2017, 121, 3142.
207. Stable colloids in molten inorganic salts
H. Zhang, K. Dasbiswas, N. B. Ludwig, G. Han, B. Lee, S. Vaikuntanathan, and D. V. Talapin. Nature 2017, 542, 328.
206. Understanding and curing structural defects in colloidal GaAs nanocrystals
V. Srivastava, W. Liu, E. M. Janke, V. Kamysbayev, A. S. Filatov, C. Sun, B. Lee, Tijana Rajh, R. D. Schaller, and D. V. Talapin. Nano Lett. 2017, 17, 2094.
205. Violet-to-Blue Gain and Lasing from Colloidal CdS Nanoplatelets: Low-Threshold Stimulated Emission Despite Low Photoluminescence Quantum Yield
B. T. Diroll, D. V. Talapin, and R. D. Schaller. ACS Photonics 2017, 4, 576.
204. New forms of CdSe: molecular wires, gels, and ordered mesoporous assemblies
M. H. Hudson, D. S. Dolzhnikov, A. S. Filatov, E. M. Janke, J. Jang, B. Lee, C. Sun, and D. V. Talapin. J. Am. Chem. Soc. 2017, 139, 3368.
203. Tandem Solar Cells from Solution-Processed CdTe and PbS Quantum Dots Using a ZnTe–ZnO Tunnel Junction
R. W. Crisp, G. F. Pach, J. M. Kurley, R. M. France, M. O. Reese, S. U. Nanayakkara, B. A. MacLeod, D. V. Talapin, M. C. Beard, and J. M. Luther. Nano Lett. 2017, 17, 1020.
202. Transparent Ohmic Contacts for Solution-Processed, Ultrathin CdTe Solar Cells
J. M. Kurley, M. G. Panthani, R. W. Crisp, S. U. Nanayakkara, G. F. Pach, M. O. Reese, M. H. Hudson, D. S. Dolzhnikov, V. Tanygin, J. M. Luther, and D. V. Talapin. ACS Energy Lett. 2017, 2, 270.