Benjamin J. Lawrie

Oak Ridge National Laboratory

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Raphael C. Pooser

Oak Ridge National Laboratory

Yun‐Yi Pai

Apple (United States)

Richard F. Haglund

Vanderbilt University

Claire E. Marvinney

Oak Ridge National Laboratory

Matthew Feldman

Quantum Science Center

Alexander A. Puretzky

Oak Ridge National Laboratory

Roderick B. Davidson

United States Naval Research Laboratory

Philip G. Evans

Oak Ridge National Laboratory

Jordan A. Hachtel

Oak Ridge National Laboratory

Alberto M. Marino

University of Oklahoma

Cooperative Institutions

Oak Ridge National Laboratory

198

University of Tennessee at Knoxville

107

Argonne National Laboratory

Quantum Science Center

Oak Ridge Associated Universities

Center for Nanophase Materials Sciences

Fermi National Accelerator Laboratory

Purdue University West Lafayette

University of Chicago

Stanford University

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Parallel Quantum-Enhanced Plasmonic Sensing

Bulletin of the American Physical Society (2019)

Aye Win Mohammadjavad Dowran Ashok Kumar Benjamin J. Lawrie Raphael C. Pooser

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High-Throughput Automated Exploration of Phase Growth Kinetics in Quasi-2D Formamidinium Metal Halide Perovskites

Jonghee Yang Benjamin J. Lawrie Sergei V. Kalinin Mahshid Ahmadi

Quasi-two-dimensional (2D) metal halide perovskites (MHPs) are an emerging material platform for sustainable functional optoelectronics, however the uncontrollable, broad phase distribution remains a critical challenge for applications. This is because the basic principles for controlling multiple phases in quasi-2D MHPs remain poorly understood, due to the rapid crystallization kinetics during the conventional thin-film fabrication process. Herein, a high-throughput automated synthesis-characterization-analysis workflow is implemented to accelerate material exploration in formamidinium (FA)-based quasi-2D MHP compositional space, revealing the early-stage phase growth kinetics which fundamentally determines the phase distributions. We observe that the prominent n=2 2D phase restricts the growth kinetics of 3D-like phases – α-FAPbI3 MHPs where the spacers are coordinated to the surface. δ-FAPbI3 phase further inhibits the growth of 3D-like phases. It is found that thermal annealing is a critical step for proper phase growth, although it can lead to the emergence of unwanted local PbI2 crystallites. Additionally, fundamental insights into the precursor chemistry associated with spacer-solvent interaction that determines the morphologies and microstructures of quasi-2D MHP films are demonstrated. Our high-throughput study provides comprehensive insights into the fundamental principles in quasi-2D MHP phase control and enables new control of the functionalities of complex materials systems for sustainable device applications.

Formamidinium

Characterization

10.26434/chemrxiv-2023-zcvl0

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Surface‐Driven Evolution of the Anomalous Hall Effect in Magnetic Topological Insulator MnBi₂Te₄ Thin Films

Advanced Functional Materials (2022)

Alessandro R. Mazza Jason Lapano Harry M. MeyerIII Christopher T. Nelson Tyler Smith

Abstract Understanding the effects of the interfacial modification to the functional properties of magnetic topological insulator thin films is crucial for developing novel technological applications from spintronics to quantum computing. Here, a large electronic and magnetic response is reported to be induced in the intrinsic magnetic topological insulator MnBi 2 Te 4 by controlling the propagation of surface oxidation. It is shown that the formation of the surface oxide layer is confined to the top 1–2 unit cells but drives large changes in the overall magnetic response. Specifically, a dramatic reversal of the sign of the anomalous Hall effect is observed to be driven by finite thickness magnetism, which indicates that the film splits into distinct magnetic layers each with a unique electronic signature. These data reveal a delicate dependence of the overall magnetic and electronic response of MnBi 2 Te 4 on the stoichiometry of the top layers. This study suggests that perturbations resulting from surface oxidation may play a non‐trivial role in the stabilization of the quantum anomalous Hall effect in this system and that understanding targeted modifications to the surface may open new routes for engineering novel topological and magnetic responses in this fascinating material.

Topological insulator

Magnetism

Stoichiometry

Surface States

10.1002/adfm.202202234

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Surface‐Driven Evolution of the Anomalous Hall Effect in Magnetic Topological Insulator MnBi₂Te₄ Thin Films (Adv. Funct. Mater. 28/2022)

Advanced Functional Materials (2022)

Alessandro R. Mazza Jason Lapano Harry M. MeyerIII Christopher T. Nelson Tyler Smith

Magnetic Topological Insulators Targeted modification of properties is crucial to engineer novel phenomena such as the quantum anomalous Hall effect. In article number 2202234, Gyula Eres, Matthew Brahlek, and co-workers show that the anomalous Hall effect in the magnetic topological insulator MnBi2Te4 is highly tunable, to the point of complete sign reversal, by modification of the top-most layer via oxidation, which is linked to a subtle rebalancing of the global magnetic state.

Topological insulator

Surface States

10.1002/adfm.202270162

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Bright and durable scintillation from colloidal quantum shells

Nature Communications (2024)

Burak Güzeltürk Benjamin T. Diroll James Cassidy Dulanjan Harankahage Muchuan Hua

Efficient, fast, and robust scintillators for ionizing radiation detection are crucial in various fields, including medical diagnostics, defense, and particle physics. However, traditional scintillator technologies face challenges in simultaneously achieving optimal performance and high-speed operation. Herein we introduce colloidal quantum shell heterostructures as X-ray and electron scintillators, combining efficiency, speed, and durability. Quantum shells exhibit light yields up to 70,000 photons MeV

10.1038/s41467-024-48351-9

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Front Cover: Magneto‐Optical Sensing Beyond the Shot Noise Limit (Adv. Quantum Technol. 1/2022)

Advanced Quantum Technologies (2022)

Yun‐Yi Pai Claire E. Marvinney Chengyun Hua Raphael C. Pooser Benjamin J. Lawrie

Classical magneto-optical microscopies are workhorse tools for materials characterization, but they are fundamentally limited in sensitivity by the photon shot noise limit. Quantum mechanical light sources guarantee that the aforementioned “standard quantum limit” is beaten. In article number 2100107, Yun-Yi Pai, Raphael C. Pooser, Benjamin J. Lawrie, and co-workers describe quantum enhanced magneto-optical Kerr effect measurements that are accessible with today's quantum optical resources – an optical parametric amplifier. This approach to quantum sensing of quantum materials enables 10 nrad/√Hz sensitivity at temperatures well below 100 mK. [Cover design by Yun-Yi Pai]

Quantum limit

Quantum noise

Quantum sensor

Quantum imaging

Quantum Metrology

10.1002/qute.202270011

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Ultrafast Surface-Plasmon Enhancement of Exciton and Defect Luminescence in ZnO Thin Films

EPJ Web of Conferences (2013)

Benjamin J. Lawrie R. Mu Richard F. Haglund

Femtosecond pump-probe and photoluminescence measurements in transmission and reflection show that ultraviolet band-edge and visible defect luminescence in ZnO films can be selectively enhanced by coupling to Ag surface-plasmon polaritons or localized surface plasmon resonances.

Localized surface plasmon

Ultraviolet

10.1051/epjconf/20134104016

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Evidence of photochromism in a hexagonal boron nitride single-photon emitter

Optica (2020)

Matthew Feldman Claire E. Marvinney Alexander A. Puretzky Benjamin J. Lawrie

Solid-state single-photon emitters (SPEs) such as the bright, stable, room-temperature defects within hexagonal boron nitride (hBN) are of increasing interest for quantum information science applications. To date, the atomic and electronic origins of SPEs within hBN are not well understood, and no studies have reported photochromism or explored cross-correlations between hBN SPEs. Here, we combine irradiation-time dependent measures of quantum efficiency and microphotoluminescence (${\mu}$PL) spectroscopy with two-color Hanbury Brown-Twiss interferometry to enable an investigation of the electronic structure of hBN defects. We identify photochromism in a hBN SPE that exhibits cross-correlations and correlated quantum efficiencies between the emission of its two zero-phonon lines.

Hexagonal boron nitride

10.1364/optica.406184

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Waveform analysis of a large-area superconducting nanowire single photon detector

Superconductor Science and Technology (2020)

Claire E. Marvinney Brian E. Lerner Alexander A. Puretzky Aaron Miller Benjamin J. Lawrie

Superconducting nanowire single photon detectors (SNSPDs) are typically used as single-mode-fiber-coupled single-pixel detectors, but large area detectors are increasingly critical for applications ranging from microscopy to free-space quantum communications. Here, we explore changes in the rising edge of the readout pulse for large-area SNSPDs as a function of the bias current, optical spot size on the detector, and number of photons per pulse. We observe a bimodal distribution of rise times and show that the probability of a slow rise time increases in the limit of large spot sizes and small photon number. In the limit of low bias currents, the dark-count readout pulse is most similar to the combined large spot size and small-photon-number bright-count readout pulse. These results are consistent with a simple model of traveling microwave modes excited by single photons incident at varying positions along the length of the nanowire.

Kinetic inductance

10.1088/1361-6668/abd150

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arXiv (Cornell University) (2021)

Jong Mok Ok Narayan Mohanta Jie Zhang Sangmoon Yoon Satoshi Okamoto

Quantum materials (QMs) with strong correlation and non-trivial topology are indispensable to next-generation information and computing technologies. Exploitation of topological band structure is an ideal starting point to realize correlated topological QMs. Herein, we report that strain-induced symmetry modification in correlated oxide SrNbO3 thin films creates an emerging topological band structure. Dirac electrons in strained SrNbO3 films reveal ultra-high mobility (100,000 cm2/Vs), exceptionally small effective mass (0.04me), and non-zero Berry phase. More importantly, strained SrNbO3 films reach the extreme quantum limit, exhibiting a sign of fractional occupation of Landau levels and giant mass enhancement. Our results suggest that symmetry-modified SrNbO3 is a rare example of a correlated topological QM, in which strong correlation of Dirac electrons leads to the realization of fractional occupation of Landau levels.

Realization (probability)

Landau quantization

Quantum limit

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