Pub Date : 2026-10-14Epub Date: 2026-09-29DOI: 10.1021/acs.nanolett.6c03033
Jae Hyun Nam, Daan Hein Alsem, Peter J. Bruggeman
Plasma-driven solutionelectrochemistry (PDSE) offers an additive-freeapproach to nanomaterial synthesis but has not been widely implementedbecause of the current lack of control strategies, rooted in the limitedmechanistic understanding of nucleation and growth that has been inaccessibleto direct observation. We report on the real-time visualization ofgold nanoparticle nucleation, growth, and coalescence in a thin ionicliquid film using a newly developed in situ plasma–liquidtransmission electron microscopy platform. Monomer attachment is identifiedas the dominant growth process, and the measured growth rates suggesta nucleation-limited regime. Trajectory analysis reveals enhancednucleation near the film edge, likely due to an increased monomerconcentration caused by plasma-induced solvent evaporation. The reportedobservations provide critical insights into mechanisms and rate-limitingprocesses and can provide guidance for PDSE-enabled process developmentto achieve the rapid synthesis of colloidal nanomaterials with a narrowsize distribution.
{"title":"In Situ Transmission Electron Microscopy of Plasma-Driven Nanoparticle Synthesis in Solution","authors":"Jae Hyun Nam, Daan Hein Alsem, Peter J. Bruggeman","doi":"10.1021/acs.nanolett.6c03033","DOIUrl":"https://doi.org/10.1021/acs.nanolett.6c03033","url":null,"abstract":"<p>Plasma-driven solutionelectrochemistry (PDSE) offers an additive-freeapproach to nanomaterial synthesis but has not been widely implementedbecause of the current lack of control strategies, rooted in the limitedmechanistic understanding of nucleation and growth that has been inaccessibleto direct observation. We report on the real-time visualization ofgold nanoparticle nucleation, growth, and coalescence in a thin ionicliquid film using a newly developed <em>in situ</em> plasma–liquidtransmission electron microscopy platform. Monomer attachment is identifiedas the dominant growth process, and the measured growth rates suggesta nucleation-limited regime. Trajectory analysis reveals enhancednucleation near the film edge, likely due to an increased monomerconcentration caused by plasma-induced solvent evaporation. The reportedobservations provide critical insights into mechanisms and rate-limitingprocesses and can provide guidance for PDSE-enabled process developmentto achieve the rapid synthesis of colloidal nanomaterials with a narrowsize distribution.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13843–13852"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14Epub Date: 2026-09-29DOI: 10.1021/acs.nanolett.6c03346
Hsiang-Ting Lin, Christine Huang, Jonah J. Ng, Christopher B. Murray, Cherie R. Kagan
Circular dichroism (CD) in plasmonic metamaterials canbe strengthenedby engineering three-dimensional (3D) chiral geometry and electromagneticcoupling. We report 3D helical-shaped plasmonic metamaterials assembledfrom colloidal Au nanocrystal/bulk Au bilayer heterostructures. Arraysof planar spiral patterns defined by nanoimprint lithography are transformedinto 3D helical metamaterials through strain-driven, out-of-planefolding induced by ligand exchange and annealing. Compared with multiple-short-arm(4C) references having the same total arm length, single-helical (1H)structures exhibit stronger differential transmittance between left-and right-handed circularly polarized light (ΔT). Adding a second helical arm to form double-helical (2H) structuresfurther increases ΔT to nearly 70% in the mid-infraredrange. Electromagnetic simulations reveal that intra-meta-atom coupling,antenna loading, and mode hybridization reshape the resonances andamplify CD beyond the response of isolated components. This work demonstratesthat 3D helical architectures can significantly strengthen plasmonicCD responses and provides a scalable nanocrystal-based platform fordesigning compact mid-infrared chiroptical devices.
{"title":"Enhanced Circular Dichroism in 3D Helical-Shaped Chiral Plasmonic Metamaterials Assembled from Colloidal Nanocrystals","authors":"Hsiang-Ting Lin, Christine Huang, Jonah J. Ng, Christopher B. Murray, Cherie R. Kagan","doi":"10.1021/acs.nanolett.6c03346","DOIUrl":"https://doi.org/10.1021/acs.nanolett.6c03346","url":null,"abstract":"<p>Circular dichroism (CD) in plasmonic metamaterials canbe strengthenedby engineering three-dimensional (3D) chiral geometry and electromagneticcoupling. We report 3D helical-shaped plasmonic metamaterials assembledfrom colloidal Au nanocrystal/bulk Au bilayer heterostructures. Arraysof planar spiral patterns defined by nanoimprint lithography are transformedinto 3D helical metamaterials through strain-driven, out-of-planefolding induced by ligand exchange and annealing. Compared with multiple-short-arm(4C) references having the same total arm length, single-helical (1H)structures exhibit stronger differential transmittance between left-and right-handed circularly polarized light (Δ<em>T</em>). Adding a second helical arm to form double-helical (2H) structuresfurther increases Δ<em>T</em> to nearly 70% in the mid-infraredrange. Electromagnetic simulations reveal that intra-meta-atom coupling,antenna loading, and mode hybridization reshape the resonances andamplify CD beyond the response of isolated components. This work demonstratesthat 3D helical architectures can significantly strengthen plasmonicCD responses and provides a scalable nanocrystal-based platform fordesigning compact mid-infrared chiroptical devices.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13913–13920"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149173940","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14Epub Date: 2026-10-05DOI: 10.1021/acs.nanolett.6c02280
Khalid N. Anindya, Hong Guo
Organic radical chains provide anatomically preciseplatform forrealizing interacting quantum spin nanostructures, but controllingthe local fate of fractional boundary degrees of freedom at internalinterfaces remains challenging. Here, we investigate interfaces betweena dimerized spin-1/2 sector and a Hund-coupled effective Haldane spin-1sector within a trioxoazatriangulene-based parent chain. Althoughthe constituent fractional boundary moments are individually established,their many-body response at the heterojunction depends sensitivelyon the bond-level termination registry. In one geometry, adjoiningspin-1/2-like boundary contributions locally compensate and quenchthe interfacial response, whereas a parity-shifted registry leavesan uncompensated localized spin-1/2-like mode. Two such internal modesof a finite embedded Haldane domain hybridize with an approximatelyexponentially decreasing splitting. The active and quenched junctionstherefore exhibit distinct local low-energy spin responses. Theseresults identify termination parity and bond-level interface registryas practical control parameters for activating, locally quenching,and coupling fractional spin modes in organic quantum spin nanostructures.
{"title":"Termination-Controlled Fractional Spin Modes at Organic Topological Spin–Chain Interfaces","authors":"Khalid N. Anindya, Hong Guo","doi":"10.1021/acs.nanolett.6c02280","DOIUrl":"10.1021/acs.nanolett.6c02280","url":null,"abstract":"<p>Organic radical chains provide anatomically preciseplatform forrealizing interacting quantum spin nanostructures, but controllingthe local fate of fractional boundary degrees of freedom at internalinterfaces remains challenging. Here, we investigate interfaces betweena dimerized spin-1/2 sector and a Hund-coupled effective Haldane spin-1sector within a trioxoazatriangulene-based parent chain. Althoughthe constituent fractional boundary moments are individually established,their many-body response at the heterojunction depends sensitivelyon the bond-level termination registry. In one geometry, adjoiningspin-1/2-like boundary contributions locally compensate and quenchthe interfacial response, whereas a parity-shifted registry leavesan uncompensated localized spin-1/2-like mode. Two such internal modesof a finite embedded Haldane domain hybridize with an approximatelyexponentially decreasing splitting. The active and quenched junctionstherefore exhibit distinct local low-energy spin responses. Theseresults identify termination parity and bond-level interface registryas practical control parameters for activating, locally quenching,and coupling fractional spin modes in organic quantum spin nanostructures.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13746–13752"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149088173","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14Epub Date: 2026-10-05DOI: 10.1021/acs.nanolett.6c02350
Benedikt Frohn, Tobias Schmitt, Vanessa Serrano, Anne Schmidt, Michael Schleenvoigt, Albert Hertel, Benjamin Bennemann, Abdur Rehman Jalil, Detlev Grützmacher, Peter Schüffelgen
Hybrid superconductor–topological insulator (TI)nanostructuresconstitute a promising material platform for exploring proximity-inducedsuperconductivity in systems with topologically protected surfacestates. A key obstacle has been the realization of clean and well-controlledsuperconductor–TI interfaces, as TI surfaces rapidly degradeunder ambient conditions. Here, we introduce a fully in situ, multi-angle stencil lithography technique that enables the fabricationof proximitized charge islands in TIs. The approach combines selectivearea growth of (Bi,Sb)2Te3 nanoribbons withangle-controlled deposition of diffusion barriers, superconductingAl, and ultrathin oxide tunnel barriers, allowing scalable fabricationof hybrid nanostructures without post-growth processing. Low-temperaturetransport measurements reveal robust Coulomb blockade and a pronouncedsuppression of low-energy conductance, which vanishes with a magneticfield, consistent with proximity-induced superconductivity in theisland. These results establish a versatile nanofabrication platformthat enables access to previously unexplored TI-based hybrid quantumdevices and opens new routes for investigating superconductivity intopological nanostructures.
{"title":"Proximitized Topological Insulator Charge Island Fabricated via In Situ Multi-Angle Stencil Lithography","authors":"Benedikt Frohn, Tobias Schmitt, Vanessa Serrano, Anne Schmidt, Michael Schleenvoigt, Albert Hertel, Benjamin Bennemann, Abdur Rehman Jalil, Detlev Grützmacher, Peter Schüffelgen","doi":"10.1021/acs.nanolett.6c02350","DOIUrl":"10.1021/acs.nanolett.6c02350","url":null,"abstract":"<p>Hybrid superconductor–topological insulator (TI)nanostructuresconstitute a promising material platform for exploring proximity-inducedsuperconductivity in systems with topologically protected surfacestates. A key obstacle has been the realization of clean and well-controlledsuperconductor–TI interfaces, as TI surfaces rapidly degradeunder ambient conditions. Here, we introduce a fully <em>in situ</em>, multi-angle stencil lithography technique that enables the fabricationof proximitized charge islands in TIs. The approach combines selectivearea growth of (Bi,Sb)<sub>2</sub>Te<sub>3</sub> nanoribbons withangle-controlled deposition of diffusion barriers, superconductingAl, and ultrathin oxide tunnel barriers, allowing scalable fabricationof hybrid nanostructures without post-growth processing. Low-temperaturetransport measurements reveal robust Coulomb blockade and a pronouncedsuppression of low-energy conductance, which vanishes with a magneticfield, consistent with proximity-induced superconductivity in theisland. These results establish a versatile nanofabrication platformthat enables access to previously unexplored TI-based hybrid quantumdevices and opens new routes for investigating superconductivity intopological nanostructures.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13753–13758"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149088175","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14Epub Date: 2026-10-03DOI: 10.1021/acs.nanolett.6c03133
Shurong Miao, I. K. M. Reaz Rahman, Aditya Nirmale, Inha Kim, Dorottya Urmossy, Thomas P. Darlington, Harishankar Jayakumar, Seiichiro Izawa, Archana Raja, Daryl C. Chrzan, Yutaka Majima, Ali Javey
Spectrally isolated,electrically driven emission fromlocalizedstates in two-dimensional semiconductors remains challenging in scalableplanar devices. Here, we report narrow-line-width alternating-currentelectroluminescence (ACEL) from localized states in monolayer WSe2 using a lithographically defined sub-5 nm Au/Pt nanogap onSiO2/Si at 3.5 K. The curved nanogap geometry producesa nonuniform strain landscape and regions of enhanced electric fieldthat may influence the local electronic environment. Under square-wavegate excitation, the device exhibits a spectrally isolated ACEL lineat 1.652 eV with an apparent fitted line width of approximately 2meV, in contrast to broad, multipeak photoluminescence from the samedevice. Spectral decomposition identifies dominant ZPL-like and weakerred-shifted sideband-like contributions. This nanogap architectureprovides a scalable planar platform for narrow-line-width, electricallydriven localized emission in two-dimensional materials.
{"title":"Narrow-Line-Width Electroluminescence in Monolayer WSe2 Enabled by a Sub-5 nm Au/Pt Nanogap","authors":"Shurong Miao, I. K. M. Reaz Rahman, Aditya Nirmale, Inha Kim, Dorottya Urmossy, Thomas P. Darlington, Harishankar Jayakumar, Seiichiro Izawa, Archana Raja, Daryl C. Chrzan, Yutaka Majima, Ali Javey","doi":"10.1021/acs.nanolett.6c03133","DOIUrl":"10.1021/acs.nanolett.6c03133","url":null,"abstract":"<p>Spectrally isolated,electrically driven emission fromlocalizedstates in two-dimensional semiconductors remains challenging in scalableplanar devices. Here, we report narrow-line-width alternating-currentelectroluminescence (ACEL) from localized states in monolayer WSe<sub>2</sub> using a lithographically defined sub-5 nm Au/Pt nanogap onSiO<sub>2</sub>/Si at 3.5 K. The curved nanogap geometry producesa nonuniform strain landscape and regions of enhanced electric fieldthat may influence the local electronic environment. Under square-wavegate excitation, the device exhibits a spectrally isolated ACEL lineat 1.652 eV with an apparent fitted line width of approximately 2meV, in contrast to broad, multipeak photoluminescence from the samedevice. Spectral decomposition identifies dominant ZPL-like and weakerred-shifted sideband-like contributions. This nanogap architectureprovides a scalable planar platform for narrow-line-width, electricallydriven localized emission in two-dimensional materials.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 40","pages":"13862–13870"},"PeriodicalIF":9.1,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149088198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-10-14DOI: 10.1021/acs.nanolett.6c03319
Ateesh K. Rathi,Rajan Singh,Javed A. Mondal,Arnab Sarkar,Ryan J. T. Nicholl,Kirill I. Bolotin,Saikat Ghosh
Abstract Nonlinear nanomechanical resonators give convenient solid-state access to classical analogs of extreme nonlinear optics and to phononic signal processing. Here we report integer harmonic generation, phononic frequency sideband comb, and reverse period-doubling dynamics in a single platform of a suspended graphene resonator. A gate voltage breaks the out-of-plane symmetry of the membrane and establishes a 1:2 internal resonance between mechanical resonators. Under a single drive tone, integer harmonics are generated sequentially, forming a dense sideband frequency comb at larger drive. Raising the drive further, we find a reverse period-doubling transition: the comb spacing doubles, the line density halves, and energy flows back into the even-order comb lines. The measured spectrum yields the quadratic (ζ) and cubic (β) nonlinear coefficients of the membrane. These results demonstrate electrical control of several nonlinear landscapes in a single graphene resonator, enabling frequency multiplication, sideband comb generation, and broadband irregular motion.
{"title":"Tunable Nonlinear\u0000Landscapes in Graphene Nanoelectromechanical\u0000Systems","authors":"Ateesh K. Rathi,Rajan Singh,Javed A. Mondal,Arnab Sarkar,Ryan J. T. Nicholl,Kirill I. Bolotin,Saikat Ghosh","doi":"10.1021/acs.nanolett.6c03319","DOIUrl":"https://doi.org/10.1021/acs.nanolett.6c03319","url":null,"abstract":"Abstract Nonlinear nanomechanical resonators give convenient solid-state access to classical analogs of extreme nonlinear optics and to phononic signal processing. Here we report integer harmonic generation, phononic frequency sideband comb, and reverse period-doubling dynamics in a single platform of a suspended graphene resonator. A gate voltage breaks the out-of-plane symmetry of the membrane and establishes a 1:2 internal resonance between mechanical resonators. Under a single drive tone, integer harmonics are generated sequentially, forming a dense sideband frequency comb at larger drive. Raising the drive further, we find a reverse period-doubling transition: the comb spacing doubles, the line density halves, and energy flows back into the even-order comb lines. The measured spectrum yields the quadratic (ζ) and cubic (β) nonlinear coefficients of the membrane. These results demonstrate electrical control of several nonlinear landscapes in a single graphene resonator, enabling frequency multiplication, sideband comb generation, and broadband irregular motion.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"14 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2026-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209320","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}