Article
Materials Science, Multidisciplinary
C. Kaspar, A. Erpenbeck, J. Baetge, C. Schinabeck, M. Thoss
Summary: The interaction between electronic and vibrational degrees of freedom has a significant impact on electron transport in molecular nanostructures, especially for nonadiabatic coupling scenarios. The study employs the numerically exact hierarchical equations of motion approach to analyze the effects and reveals a variety of interesting transport phenomena.
Article
Materials Science, Multidisciplinary
Ashima Bajaj, Rishu Khurana, Md Ehesan Ali
Summary: A stimuli-based spin filter using a photo-responsive endoperoxide (EPO) based single molecule device has been developed, with the diradical intermediate of EPO facilitating high spin filtering efficiency. The transmission characteristics of various photoproducts along the photochemical reaction pathway of EPO are investigated, demonstrating the key role of quantum interference effects in the modulation of conductance.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Chemistry, Multidisciplinary
Liang Li, Jonathan Z. Low, Jan Wilhelm, Guanming Liao, Suman Gunasekaran, Claudia R. Prindle, Rachel L. Starr, Dorothea Golze, Colin Nuckolls, Michael L. Steigerwald, Ferdinand Evers, Luis M. Campos, Xiaodong Yin, Latha Venkataraman
Summary: A family of oligophenylene-bridged bis(triarylamines) with tunable and stable mono- or di-radicaloid character was studied, showing reversed conductance decay with increasing length for oxidized wires, indicating non-classical quasi-metallic behavior.
Article
Chemistry, Multidisciplinary
Mingpeng Chen, Andrew C. Grieder, Tyler J. Smart, Kiley Mayford, Samuel McNair, Anica Pinongcos, Samuel Eisenberg, Frank Bridges, Yat Li, Yuan Ping
Summary: Hematite, a transition metal oxide, has the advantages of low cost, high abundance, and good chemical stability, making it a promising material for energy conversion and storage applications. However, its low carrier mobility and electrical conductivity have limited its widespread application. Atomic doping has been considered as a promising approach to improve its electrical conductivity, but the impact on carrier mobility at the atomic level has remained unclear. In this study, we used a kinetic Monte-Carlo sampling approach to calculate the electrical conductivity of doped hematite and investigated how different dopants affect carrier mobility. Our results showed that the local distortion of Fe-Fe pairs caused by dopants is closely related to the change in carrier mobility. Elements that minimize the distortion of Fe-Fe pairs are preferred for higher carrier mobility in hematite. The accuracy of our predictions was further validated by experimental measurements. This work provides practical guidelines for experimentalists on choosing dopants to optimize the electrical conductivity and performance of hematite-based devices.
Article
Chemistry, Multidisciplinary
Michael Yannai, Raphael Dahan, Alexey Gorlach, Yuval Adiv, Kangpeng Wang, Ivan Madan, Simone Gargiulo, Francesco Barantani, Eduardo J. C. Dias, Giovanni Maria Vanacore, Nicholas Rivera, Fabrizio Carbone, F. Javier Garcia de Abajo, Ido Kaminer
Summary: The ultrafast dynamics of charge carriers in solids is crucial for emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, investigating and visualizing such nonequilibrium phenomena at nanometer-femtosecond scales has been a longstanding challenge. In this study, we propose and demonstrate a new interaction mechanism called charge dynamics electron microscopy (CDEM), which enables nanoscale imaging of the femtosecond dynamics of charge carriers in solids. By exploiting the strong interaction of free-electron pulses with terahertz (THz) near fields created by moving charges, we can directly retrieve the THz near-field amplitude and phase, reconstruct movies of the generated charges, and investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids.
Article
Chemistry, Physical
Henning Kirchberg, Abraham Nitzan
Summary: This study considers a molecular junction immersed in a solvent, where the electron transfer occurs through Marcus-type steps. It is found that although the charge transfer is continuous, the solvent does not reach thermal equilibrium throughout the transport. By investigating the nonequilibrium solvent dynamics, the electrical, thermal, and thermoelectric properties of the molecular junction are examined. The results show that by tuning the friction, heat dissipation into the solvent can be reduced and heat transfer between the electrodes can be enhanced.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Hui-Min Wang, Xin-Bao Liu, Shi-Qi Hu, Da-Qiang Chen, Qing Chen, Cui Zhang, Meng-Xue Guan, Sheng Meng
Summary: Laser-controlled coherent phonon excitation significantly enhances carrier mobility by accelerating polaron transport. Selective excitation of specific phonon modes that overlap with the polaronic lattice deformation can reduce the energy barrier for polaron hopping. Nonadiabatic couplings between the electronic and ionic subsystems promote polaron migration through phonon-phonon scattering.
Article
Chemistry, Physical
Ondrej Dyck, Sinchul Yeom, Sarah Dillender, Andrew R. Lupini, Mina Yoon, Stephen Jesse
Summary: Graphene has unique properties such as ballistic transport, spin selectivity, quantum hall effect, etc., making it of great scientific interest. Nanopatterning and atomic scale modifications of graphene can further control its properties, including electronic properties and defect evolution.
Article
Chemistry, Multidisciplinary
Jack W. Jordan, Beth Mortiboy, Andrei N. Khlobystov, Lee R. Johnson, Graham N. Newton, Darren A. Walsh
Summary: Understanding ion transport in solid materials is crucial for the design of electrochemical devices. This study focuses on investigating ion transport across atomically thin structures using a host-guest hybrid redox material based on polyoxometalates (POMs) encapsulated within single-walled carbon nanotubes (SWNTs). The nanotube sidewall acts as a barrier between the redox-active molecules and bulk electrolytes, allowing for the characterization of ion transport through electrochemical methods. The findings highlight the importance of the nature of the cation in the supporting electrolyte and the role of proton transport in the redox chemistry of nanoconfined redox materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Physics, Applied
Juliana M. da Silva, Fernando A. F. Santana, Jorge G. G. S. Ramos, Anderson L. R. Barbosa
Summary: In this study, we investigate the behavior of the spin Hall effect in a system with disorder and interface-induced spin-orbit coupling by experimental and numerical simulations of single-layer graphene devices. The results show that the spin Hall angle of graphene devices exhibits mesoscopic fluctuations and follows a universal relationship with the dimensionless longitudinal conductivity.
JOURNAL OF APPLIED PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Zhixin Chen, Lijue Chen, Guopeng Li, Yaorong Chen, Chun Tang, Longyi Zhang, Jiangpeng Liu, Lina Chen, Yang Yang, Jia Shi, Junyang Liu, Haiping Xia, Wenjing Hong
Summary: By introducing intramolecular hydrogen bonds through modification of two hydroxyls, the conductance of single-molecule junctions with a meta-connected benzene ring is enhanced by about 45 times, leading to the transition from through-bond to through-space transport as observed from flicker noise analysis. The significant difference in charge transport is originated from the blocking of transmission path due to Jahn-Teller distortion, resulting in the disappearance of destructive quantum interference feature in both experimental and theoretical results.
CELL REPORTS PHYSICAL SCIENCE
(2021)
Review
Nanoscience & Nanotechnology
Hongliang Chen, Chuancheng Jia, Xin Zhu, Chen Yang, Xuefeng Guo, J. Fraser Stoddart
Summary: Developing new materials is a long-standing goal in various fields, and understanding single-molecule reactions can deepen our understanding of chemical reactions and provide new frameworks in materials science. This review focuses on state-of-the-art chemical reactions in single-molecule junctions and highlights the advantages of real-time testbeds for studying reaction dynamics, intermediates, transition states, and solvent effects. The behavior of single-molecule reactions is compared with reactions in ensemble states, and the potential of leveraging single-molecule catalysis for large-scale materials production is explored.
NATURE REVIEWS MATERIALS
(2023)
Article
Chemistry, Physical
S. Aria Hosseini, Giuseppe Romano, P. Alex Greaney
Summary: The addition of porosity to thermoelectric materials can enhance the figure of merit ZT by reducing thermal conductivity, but also has detrimental effects on the power factor. By fine tuning carrier concentration and designing pore size and shape, electrical performance in nanoporous Si can be optimized. Cubic pores show the largest enhancement in Seebeck coefficient, with potential improvements of up to 60% at high carrier populations.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Tao He, C. Daniel Frisbie
Summary: Electric double layer transistors (EDLTs) based on C-60 single crystals and ionic liquid gates show pronounced peaks in sheet conductance versus gate-induced charge, and the choice of ionic liquid cation has a significant impact on the conductance suppression.
Review
Chemistry, Multidisciplinary
Shijie Liang, Xudong Jiang, Chengyi Xiao, Cheng Li, Qiaomei Chen, Weiwei Li
Summary: Double-cable conjugated polymers have shown potential in organic solar cells, but face challenges such as limited chemical structures and difficulty in morphology tuning. Some novel double-cable conjugated polymers have achieved a high power conversion efficiency of 8.4%, representing a new breakthrough for SCOSCs devices.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Makars Siskins, Ekaterina Sokolovskaya, Martin Lee, Samuel Manas-Valero, Dejan Davidovikj, Herre S. J. van der Zant, Peter G. Steeneken
Summary: Coupled nanomechanical resonators made of two-dimensional materials show promise for information processing, but controlling the coupling is a challenge. This study demonstrates strong coupling of motion between suspended membranes of magnetic 2D material FePS3 and introduces a tunable electromechanical mechanism for controlling both frequency and coupling strength. The potential of this electrical coupling in transferring mechanical energy over a distance at low electrical power for novel data readout and information processing technologies is highlighted.
Article
Chemistry, Multidisciplinary
Martin Lee, Martin P. Robin, Ruben H. Guis, Ulderico Filippozzi, Dong Hoon Shin, Thierry C. van Thiel, Stijn P. Paardekooper, Johannes R. Renshof, Herre S. J. van der Zant, Andrea D. Caviglia, Gerard J. Verbiest, Peter G. Steeneken
Summary: This work demonstrates the use of self-sealing membranes to seal the reference cavity beneath, improving the gas permeation time constant. The adhesion increase over SiO2 is mediated by oxygen bonds that are formed at the SiO2/complex oxide interface during the self-sealing anneal.
Article
Chemistry, Multidisciplinary
Werner M. Schosser, Chunwei Hsu, Patrick Zwick, Katawoura Beltako, Diana Dulic, Marcel Mayor, Herre S. J. van der Zant, Fabian Pauly
Summary: The study investigates quantum interference phenomena in molecular electronics at ambient conditions by connecting two porphyrins and mechanically controlling electric transport. The combination of experimental and theoretical methods reveals variations in electrical conductivity during molecular stretching and confirms the mechanosensitive response of molecular junctions. The study also observes uncommon frequency responses in periodic electrode modulation experiments, further confirming predicted transmission dips caused by rearrangement of molecular orbitals.
Article
Chemistry, Physical
Frederik H. van Veen, Luca Ornago, Herre S. J. van der Zant, Maria El Abbassi
Summary: This study investigates the variation in conductance values of alkanes using the mechanically controlled break junction technique. By analyzing the time evolution and distance dependence of the measured traces, the single-molecule conductance values for fully stretched molecular configurations are determined. The results provide crucial information for determining the molecular junction configuration.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Physics, Multidisciplinary
Chunwei Hsu, Theo A. Costi, David Vogel, Christina Wegeberg, Marcel Mayor, Herre S. J. van der Zant, Pascal Gehring
Summary: Probing the universal low-temperature magnetic field scaling of Kondo-correlated quantum dots via electrical conductance has proven to be experimentally challenging. In this study, we demonstrate how to probe this phenomenon using nonlinear thermocurrent spectroscopy applied to a molecular quantum dot in the Kondo regime. Our findings show that bias-dependent thermocurrent is a sensitive probe of the universal Kondo physics, allowing for direct measurement of the splitting of the Kondo resonance in a magnetic field, and opening up possibilities for investigating nanosystems far from thermal and electrical equilibrium.
PHYSICAL REVIEW LETTERS
(2022)
Article
Chemistry, Physical
Luca Ornago, Jerry Kamer, Maria El Abbassi, Ferdinand C. Grozema, Herre S. J. van der Zant
Summary: Switching effects play a crucial role in the design and characterization of nanoscale molecular electronics systems. This study investigates the presence of switching events in reference molecular systems and highlights the importance of proper anchoring group selection and comparison with reference compounds in understanding the origin of switching in molecular break junctions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Abdalghani Daaoub, Luca Ornago, David Vogel, Pablo Bastante, Sara Sangtarash, Matteo Parmeggiani, Jerry Kamer, Hatef Sadeghi, Herre van der Zant, Marcel Mayor, Nicolas Agrait
Summary: This study investigates the influence of side groups on charge transport through single molecules and demonstrates the ability of side groups to modulate the energy levels of transport orbitals. A novel statistical method to predict the electrical conductance of molecular junctions is also proposed.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Thomas Y. Baum, Saleta Fern andez, Diego Pen, Herre S. J. van der Zant
Summary: In this study, charge-transport experiments with bianthracene-based radicals were conducted at low temperatures. It was found that the magnetism of the diradical is preserved in solid-state devices and can be observed through Kondo resonance or inelastic electron tunneling spectroscopy. The exact molecular configuration in the junction affects the magnetic fingerprints. This research provides insights into the spin-spin interaction in solid-state devices and suggests the possibility of electrical or mechanical control.
Article
Physics, Applied
Katsuhiko Nishiguchi, Hiroshi Yamaguchi, Akira Fujiwara, Herre S. J. van der Zant, Gary A. Steele
Summary: We have demonstrated charge detection with single-electron resolution at high readout frequency using a silicon field-effect transistor integrated with double resonant circuits. The transistor, with a channel width of 10 nm, can detect a single electron at room temperature. The transistor is connected to resonant circuits composed of coupled inductors and capacitors, providing two resonance frequencies. By driving the transistor with a carrier signal at the lower resonance frequency, a small signal applied to the transistor's gate modulates the resonance condition, resulting in a reflected signal appearing near the higher resonance frequency. This operation allows for charge detection with a single-electron resolution of 3 x 10(-3) e/Hz(0.5) and a readout frequency of 200 MHz at room temperature.
APPLIED PHYSICS LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Amit S. Pawbake, Ruchita T. Khare, Joshua O. Island, Eduardo Flores, Jose R. Ares, Carlos Sanchez, Isabel J. Ferrer, Mahendra Pawar, Otakar Frank, Mahendra A. More, Herre S. J. van der Zant, Andres Castellanos-Gomez, Dattatray J. Late
Summary: The field emission properties of TiS3 nanosheets and nanoribbons synthesized from bulk titanium were investigated. The nanosheets exhibited enhanced field emission behavior with a low turn-on field and delivered a large emission current density at a relatively low applied electric field. The superior field emission performance of TiS3 nanosheets over nanoribbons makes them a propitious field emitter for vacuum nanoelectronics devices.
ACS APPLIED NANO MATERIALS
(2023)
Article
Physics, Applied
Serhii Volosheniuk, Damian Bouwmeester, Chunwei Hsu, H. S. J. van der Zant, Pascal Gehring
Summary: Thermocurrent flowing through a single-molecule device provides valuable information about its quantum properties, electronic and phononic excitation spectra, and entropy. Experimentally measuring the thermoelectric heat-to-charge conversion efficiency can help select suitable molecules for highly efficient energy conversion devices predicted by theoretical studies. A superconductor-normal metal-superconductor Josephson junction thermometer is incorporated into the single-molecule device to accurately determine the temperature bias. This device architecture enables precise thermoelectric experiments on individual molecules at millikelvin temperatures.
APPLIED PHYSICS LETTERS
(2023)
Article
Physics, Applied
Chunwei Hsu, Michael Rohde, Gabriela Borin Barin, Guido Gandus, Daniele Passerone, Mathieu Luisier, Pascal Ruffieux, Roman Fasel, Herre S. J. van der Zant, Maria El Abbassi
Summary: Creating a good contact between electrodes and graphene nanoribbons (GNRs) has been a long-standing challenge in the search for the next generation GNR-based nanoelectronics. This study successfully transfers armchair-edged GNRs grown on Au(111)/mica substrates to pre-patterned platinum electrodes, resulting in polymer-free field-effect transistor devices. The devices exhibit significantly lower resistance compared to previous reports, and density functional theory calculations show that platinum has strong coupling and higher transmission compared to graphene.
APPLIED PHYSICS LETTERS
(2023)
Article
Physics, Multidisciplinary
Mattias Matthiesen, Jorrit R. Hortensius, Samuel Manas-Valero, Itzik Kapon, Dumitru Dumcenco, Enrico Giannini, Makars Siskin, Boris A. Ivanov, Herre S. J. van der Zant, Eugenio Coronado, Alexey B. Kuzmenko, Dmytro Afanasiev, Andrea D. Caviglia
Summary: The research focuses on investigating optical methods for generating coherent magnons in antiferromagnetic insulators. It is found that orbital transitions are key targets for magnetic control in insulators with zero orbital angular momentum.
PHYSICAL REVIEW LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Gabriele Baglioni, Roberto Pezone, Sten Vollebregt, Katarina Cvetanovic Zobenica, Marko Spasenovic, Dejan Todorovic, Hanqing Liu, Gerard J. Verbiest, Herre S. J. van der Zant, Peter G. Steeneken
Summary: This study investigates the acoustic response of suspended graphene membranes for microphone applications using laser vibrometry. It demonstrates superior mechanical sensitivities and a lower limit of detection compared to current MEMS microphones.
Article
Chemistry, Multidisciplinary
Chunwei Hsu, Werner M. Schosser, Patrick Zwick, Diana Dulic, Marcel Mayor, Fabian Pauly, Herre S. J. van der Zant
Summary: This article reports a method to probe and control intra- and intermolecular interactions in a single molecule using conductance measurement. The experimental results show an exceptional exponential rise in conductance response by two orders of magnitude. The theoretical study explains the observed behavior by mechanical activation and strengthening of through-bond transport and through-space coupling.
