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  1. Artikel ; Online: The persistence of memory in ionic conduction probed by nonlinear optics.

    Poletayev, Andrey D / Hoffmann, Matthias C / Dawson, James A / Teitelbaum, Samuel W / Trigo, Mariano / Islam, M Saiful / Lindenberg, Aaron M

    Nature

    2024  Band 625, Heft 7996, Seite(n) 691–696

    Abstract: Predicting practical rates of transport in condensed phases enables the rational design of materials, devices and processes. This is especially critical to developing low-carbon energy technologies such as rechargeable ... ...

    Abstract Predicting practical rates of transport in condensed phases enables the rational design of materials, devices and processes. This is especially critical to developing low-carbon energy technologies such as rechargeable batteries
    Sprache Englisch
    Erscheinungsdatum 2024-01-24
    Erscheinungsland England
    Dokumenttyp Journal Article
    ZDB-ID 120714-3
    ISSN 1476-4687 ; 0028-0836
    ISSN (online) 1476-4687
    ISSN 0028-0836
    DOI 10.1038/s41586-023-06827-6
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  2. Artikel ; Online: Publisher Correction: The persistence of memory in ionic conduction probed by nonlinear optics.

    Poletayev, Andrey D / Hoffmann, Matthias C / Dawson, James A / Teitelbaum, Samuel W / Trigo, Mariano / Islam, M Saiful / Lindenberg, Aaron M

    Nature

    2024  Band 626, Heft 7999, Seite(n) E14

    Sprache Englisch
    Erscheinungsdatum 2024-01-28
    Erscheinungsland England
    Dokumenttyp Published Erratum
    ZDB-ID 120714-3
    ISSN 1476-4687 ; 0028-0836
    ISSN (online) 1476-4687
    ISSN 0028-0836
    DOI 10.1038/s41586-024-07124-6
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  3. Artikel ; Online: In Situ X-ray Scattering Reveals Coarsening Rates of Superlattices Self-Assembled from Electrostatically Stabilized Metal Nanocrystals Depend Nonmonotonically on Driving Force.

    Tanner, Christian P N / Utterback, James K / Portner, Joshua / Coropceanu, Igor / Das, Avishek / Tassone, Christopher J / Teitelbaum, Samuel W / Limmer, David T / Talapin, Dmitri V / Ginsberg, Naomi S

    ACS nano

    2024  

    Abstract: Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with promising functionalities. Mechanistic studies are still needed to uncover the design principles for SL self- ...

    Abstract Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with promising functionalities. Mechanistic studies are still needed to uncover the design principles for SL self-assembly, but such studies have been difficult to perform due to the fast time and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure the evolving phases
    Sprache Englisch
    Erscheinungsdatum 2024-02-06
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ISSN 1936-086X
    ISSN (online) 1936-086X
    DOI 10.1021/acsnano.3c12186
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  4. Buch ; Online: In situ coherent X-ray scattering reveals polycrystalline structure and discrete annealing events in strongly-coupled nanocrystal superlattices

    Hurley, Matthew J. / Tanner, Christian P. N. / Portner, Joshua / Utterback, James K. / Coropceanu, Igor / Williams, Garth J. / Das, Avishek / Fluerasu, Andrei / Sun, Yanwen / Song, Sanghoon / Hamerlynck, Leo M. / Miller, Alexander H. / Bhattacharyya, Priyadarshini / Talapin, Dmitri V. / Ginsberg, Naomi S. / Teitelbaum, Samuel W.

    2024  

    Abstract: Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong ... ...

    Abstract Solution-phase bottom up self-assembly of nanocrystals into superstructures such as ordered superlattices is an attractive strategy to generate functional materials of increasing complexity, including very recent advances that incorporate strong interparticle electronic coupling. While the self-assembly kinetics in these systems have been elucidated and related to the product characteristics, the weak interparticle bonding interactions suggest the superstructures formed could continue to order within the solution long after the primary nucleation and growth have occurred, even though the mechanism of annealing remains to be elucidated. Here, we use a combination of Bragg coherent diffractive imaging and X-ray photon correlation spectroscopy to create real-space maps of supercrystalline order along with a real-time view of the strain fluctuations in aging strongly coupled nanocrystal superlattices while they remain suspended and immobilized in solution. By combining the results, we deduce that the self-assembled superstructures are polycrystalline, initially comprising multiple nucleation sites, and that shear avalanches at grain boundaries continue to increase crystallinity long after growth has substantially slowed. This multimodal approach should be generalizable to characterize a breadth of materials in situ in their native chemical environments, thus extending the reach of high-resolution coherent X-ray characterization to the benefit of a much wider range of physical systems.

    Comment: 26 pages, 20 figures
    Schlagwörter Condensed Matter - Materials Science ; Condensed Matter - Mesoscale and Nanoscale Physics ; Condensed Matter - Soft Condensed Matter
    Erscheinungsdatum 2024-01-11
    Erscheinungsland us
    Dokumenttyp Buch ; Online
    Datenquelle BASE - Bielefeld Academic Search Engine (Lebenswissenschaftliche Auswahl)

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  5. Artikel ; Online: Dynamics of a Persistent Insulator-to-Metal Transition in Strained Manganite Films.

    Teitelbaum, Samuel W / Ofori-Okai, B K / Cheng, Yu-Hsiang / Zhang, Jingdi / Jin, Feng / Wu, Wenbin / Averitt, Richard D / Nelson, Keith A

    Physical review letters

    2020  Band 123, Heft 26, Seite(n) 267201

    Abstract: Transition metal oxides possess complex free-energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained La_{0.67}Ca_{0.33}MnO_{3}, optical excitation with a sub-100-fs pulse ... ...

    Abstract Transition metal oxides possess complex free-energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained La_{0.67}Ca_{0.33}MnO_{3}, optical excitation with a sub-100-fs pulse above 2  mJ/cm^{2} leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multistep process. We conclude that the phase transition is driven by partial charge-order melting, followed by growth of the persistent metallic phase on longer timescales. A time-dependent Ginzburg-Landau model can describe the fast dynamics of the reflectivity, followed by longer timescale in-growth of the metallic phase.
    Sprache Englisch
    Erscheinungsdatum 2020-01-22
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 208853-8
    ISSN 1079-7114 ; 0031-9007
    ISSN (online) 1079-7114
    ISSN 0031-9007
    DOI 10.1103/PhysRevLett.123.267201
    Datenquelle MEDical Literature Analysis and Retrieval System OnLINE

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  6. Buch ; Online: In situ X-ray scattering reveals coarsening rates of superlattices self-assembled from electrostatically stabilized metal nanocrystals depend non-monotonically on driving force

    Tanner, Christian P. N. / Utterback, James K. / Portner, Joshua / Coropceanu, Igor / Das, Avishek / Tassone, Christopher J. / Teitelbaum, Samuel W. / Limmer, David T. / Talapin, Dmitri V. / Ginsberg, Naomi S.

    2023  

    Abstract: Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with new functionalities. Mechanistic studies are still needed to uncover the design principles for SL self- ... ...

    Abstract Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with new functionalities. Mechanistic studies are still needed to uncover the design principles for SL self-assembly, but such studies have been difficult to perform due to the fast time- and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure the evolving phases \textit{in situ} and in real time of an electrostatically stabilized Au NC solution before, during, and after it is quenched to form SLs using small angle X-ray scattering (SAXS). By developing a quantitative model, we fit the time-dependent scattering patterns to obtain the phase diagram of the system and the kinetics of the colloidal and SL phases as a function of varying quench conditions. The extracted phase diagram is consistent with particles whose interactions are short in range relative to their diameter. We find the degree of SL order is primarily determined by fast (sub-second) initial nucleation and growth kinetics, while coarsening at later times depends non-monotonically on the driving force for self-assembly. We validate these results by direct comparison with simulations and use them to suggest dynamic design principles to optimize crystallinity within a finite time window. The combination of this measurement methodology, quantitative analysis, and simulation should be generalizable to elucidate and better control the microscopic self-assembly pathways of a wide range of bottom-up assembled systems and architectures.
    Schlagwörter Condensed Matter - Soft Condensed Matter
    Thema/Rubrik (Code) 612
    Erscheinungsdatum 2023-12-11
    Erscheinungsland us
    Dokumenttyp Buch ; Online
    Datenquelle BASE - Bielefeld Academic Search Engine (Lebenswissenschaftliche Auswahl)

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  7. Buch ; Online: The Persistence of Memory in Ionic Conduction Probed by Nonlinear Optics

    Poletayev, Andrey D. / Hoffmann, Matthias C. / Dawson, James A. / Teitelbaum, Samuel W. / Trigo, Mariano / Islam, M. Saiful / Lindenberg, Aaron M.

    2021  

    Abstract: Predicting practical rates of ion transport from atomistic descriptors enables the rational design of materials, devices, and processes, which is especially critical to developing low-carbon energy technologies such as rechargeable batteries. The ... ...

    Abstract Predicting practical rates of ion transport from atomistic descriptors enables the rational design of materials, devices, and processes, which is especially critical to developing low-carbon energy technologies such as rechargeable batteries. The correlated mechanisms of ionic conduction, variation of conductivity with timescale and confinement, and ambiguity in the vibrational origin of translation, the attempt frequency, call for a direct atomic probe of the most fundamental steps of ionic diffusion: ion hops. However, such hops are rare-event large-amplitude translations, and are challenging to excite and detect. Here we use single-cycle terahertz pumps to impulsively trigger ionic hopping in battery solid electrolytes. This is visualized by an induced transient birefringence enabling direct probing of anisotropy in ionic hopping on the picosecond timescale. The relaxation of the transient signal measures the decay of orientational memory, and the production of entropy in diffusion. We extend experimental results using in silico transient birefringence to identify attempt frequencies for ion hopping. Using nonlinear optical methods, we probe ion transport at its fastest limit, distinguish correlated conduction mechanisms from a true random walk at the atomic scale, and demonstrate the connection between activated transport and the thermodynamics of information.

    Comment: 41 pages, 22 figures
    Schlagwörter Condensed Matter - Materials Science ; Condensed Matter - Statistical Mechanics ; Physics - Chemical Physics ; Physics - Computational Physics ; Physics - Optics
    Thema/Rubrik (Code) 612
    Erscheinungsdatum 2021-10-13
    Erscheinungsland us
    Dokumenttyp Buch ; Online
    Datenquelle BASE - Bielefeld Academic Search Engine (Lebenswissenschaftliche Auswahl)

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  8. Artikel ; Online: Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals.

    Coropceanu, Igor / Janke, Eric M / Portner, Joshua / Haubold, Danny / Nguyen, Trung Dac / Das, Avishek / Tanner, Christian P N / Utterback, James K / Teitelbaum, Samuel W / Hudson, Margaret H / Sarma, Nivedina A / Hinkle, Alex M / Tassone, Christopher J / Eychmüller, Alexander / Limmer, David T / Olvera de la Cruz, Monica / Ginsberg, Naomi S / Talapin, Dmitri V

    Science (New York, N.Y.)

    2022  Band 375, Heft 6587, Seite(n) 1422–1426

    Abstract: Colloidal nanocrystals of metals, semiconductors, and other functional materials can self-assemble into long-range ordered crystalline and quasicrystalline phases, but insulating organic surface ligands prevent the development of collective electronic ... ...

    Abstract Colloidal nanocrystals of metals, semiconductors, and other functional materials can self-assemble into long-range ordered crystalline and quasicrystalline phases, but insulating organic surface ligands prevent the development of collective electronic states in ordered nanocrystal assemblies. We reversibly self-assembled colloidal nanocrystals of gold, platinum, nickel, lead sulfide, and lead selenide with conductive inorganic ligands into supercrystals exhibiting optical and electronic properties consistent with strong electronic coupling between the constituent nanocrystals. The phase behavior of charge-stabilized nanocrystals can be rationalized and navigated with phase diagrams computed for particles interacting through short-range attractive potentials. By finely tuning interparticle interactions, the assembly was directed either through one-step nucleation or nonclassical two-step nucleation pathways. In the latter case, the nucleation was preceded by the formation of two metastable colloidal fluids.
    Sprache Englisch
    Erscheinungsdatum 2022-03-24
    Erscheinungsland United States
    Dokumenttyp Journal Article ; Research Support, Non-U.S. Gov't
    ZDB-ID 128410-1
    ISSN 1095-9203 ; 0036-8075
    ISSN (online) 1095-9203
    ISSN 0036-8075
    DOI 10.1126/science.abm6753
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  9. Artikel ; Online: Extended two-temperature model for ultrafast thermal response of band gap materials upon impulsive optical excitation.

    Shin, Taeho / Teitelbaum, Samuel W / Wolfson, Johanna / Kandyla, Maria / Nelson, Keith A

    The Journal of chemical physics

    2015  Band 143, Heft 19, Seite(n) 194705

    Abstract: Thermal modeling and numerical simulations have been performed to describe the ultrafast thermal response of band gap materials upon optical excitation. A model was established by extending the conventional two-temperature model that is adequate for ... ...

    Abstract Thermal modeling and numerical simulations have been performed to describe the ultrafast thermal response of band gap materials upon optical excitation. A model was established by extending the conventional two-temperature model that is adequate for metals, but not for semiconductors. It considers the time- and space-dependent density of electrons photoexcited to the conduction band and accordingly allows a more accurate description of the transient thermal equilibration between the hot electrons and lattice. Ultrafast thermal behaviors of bismuth, as a model system, were demonstrated using the extended two-temperature model with a view to elucidating the thermal effects of excitation laser pulse fluence, electron diffusivity, electron-hole recombination kinetics, and electron-phonon interactions, focusing on high-density excitation.
    Sprache Englisch
    Erscheinungsdatum 2015-11-21
    Erscheinungsland United States
    Dokumenttyp Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
    ZDB-ID 3113-6
    ISSN 1089-7690 ; 0021-9606
    ISSN (online) 1089-7690
    ISSN 0021-9606
    DOI 10.1063/1.4935366
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  10. Artikel ; Online: Ultrafast X-Ray Scattering Reveals Composite Amplitude Collective Mode in the Weyl Charge Density Wave Material (TaSe_{4})_{2}I.

    Nguyen, Quynh L / Duncan, Ryan A / Orenstein, Gal / Huang, Yijing / Krapivin, Viktor / de la Peña, Gilberto / Ornelas-Skarin, Chance / Reis, David A / Abbamonte, Peter / Bettler, Simon / Chollet, Matthieu / Hoffmann, Matthias C / Hurley, Matthew / Kim, Soyeun / Kirchmann, Patrick S / Kubota, Yuya / Mahmood, Fahad / Miller, Alexander / Osaka, Taito /
    Qu, Kejian / Sato, Takahiro / Shoemaker, Daniel P / Sirica, Nicholas / Song, Sanghoon / Stanton, Jade / Teitelbaum, Samuel W / Tilton, Sean E / Togashi, Tadashi / Zhu, Diling / Trigo, Mariano

    Physical review letters

    2023  Band 131, Heft 7, Seite(n) 76901

    Abstract: We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe_{4})_{2}I following ultrafast infrared photoexcitation. From the time-dependent diffraction signal at the CDW sidebands we identify a 0.11 THz ... ...

    Abstract We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe_{4})_{2}I following ultrafast infrared photoexcitation. From the time-dependent diffraction signal at the CDW sidebands we identify a 0.11 THz amplitude mode derived primarily from a transverse acoustic mode of the high-symmetry structure. From our measurements we determine that this mode interacts with the valence charge indirectly through another collective mode, and that the CDW system in (TaSe_{4})_{2}I has a composite nature supporting multiple dynamically active structural degrees of freedom.
    Sprache Englisch
    Erscheinungsdatum 2023-09-01
    Erscheinungsland United States
    Dokumenttyp Journal Article
    ZDB-ID 208853-8
    ISSN 1079-7114 ; 0031-9007
    ISSN (online) 1079-7114
    ISSN 0031-9007
    DOI 10.1103/PhysRevLett.131.076901
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