-
A Unified Description of Electron-Phonon Coupling and Ion Migration in Metal Halide Perovskites
Authors:
Bo Cai,
Yan Yang,
Yoshiki Sugai,
Maddison Wiles,
Dongxu He,
Yang Yang,
Junmin Xia,
Shufen Chen,
Carla Verdi,
Siyu Chen,
Nan Zhang,
Ming-Gang Ju,
Chao Liang,
Julian A. Steele
Abstract:
The remarkable optoelectronic properties of metal halide perovskites are closely linked to their unusually soft and polar chemical bonds that enable both strong electron-phonon interactions and ion migration. Yet these two defining characteristics have largely been treated as independent consequences of the same underlying chemical bonding. Here we show that they originate from a common electronic…
▽ More
The remarkable optoelectronic properties of metal halide perovskites are closely linked to their unusually soft and polar chemical bonds that enable both strong electron-phonon interactions and ion migration. Yet these two defining characteristics have largely been treated as independent consequences of the same underlying chemical bonding. Here we show that they originate from a common electronic-structure framework by developing a general description linking lattice dynamics, electron-phonon coupling, and halide ion migration across representative Pb-based, Sn-based, and double perovskites. Spectrally resolved phonon-mode contributions demonstrate that the low-frequency shearing modes dominate halide migration, whereas high-frequency stretching modes govern carrier scattering through the Fröhlich interaction in all three compositions. We introduce an orbital hybridization descriptor to unify these findings, which connects metal-halide bonding characteristics with the migration barrier energies and Fröhlich coupling strengths, indicating a cooperative evolution of these two properties. These findings provide a generalized microscopic mechanism for simultaneously optimizing charge and ionic transport in soft semiconductors.
△ Less
Submitted 12 August, 2026;
originally announced August 2026.
-
Electron transport in a 1.6~nm-thick double-gated (100) silicon nanosheet: A theoretical study accounting for phonon confinement and remote-phonon scattering
Authors:
Shoaib Mansoori,
Bimin Cai,
Edward Chen,
Dallin O. Nielsen,
Massimo V. Fischetti
Abstract:
We study theoretically electron transport in an top-and bottom-gated (100) 1.6 nm-thin silicon nanosheet with SiO2/HfO2 gate stacks, focusing on the intrinsic physical processes that affect transport: the confinement of phonons and the presence of interface hybrid plasmon-phonon excitations (IPPs or `remote phonons'). The band structure is calculated using local empirical pseudopotentials; an appr…
▽ More
We study theoretically electron transport in an top-and bottom-gated (100) 1.6 nm-thin silicon nanosheet with SiO2/HfO2 gate stacks, focusing on the intrinsic physical processes that affect transport: the confinement of phonons and the presence of interface hybrid plasmon-phonon excitations (IPPs or `remote phonons'). The band structure is calculated using local empirical pseudopotentials; an approximated elastic continuum model is used to consider the confinement of acoustic phonons; the dielectric continuum limit is used to deal with the IPPs. We find that the electron mobility is affected significantly by the boundary conditions chosen to deal with phonon confinement. The more realistic assumption of phonons clamped at the SiO2/HfO2 interfaces and optical phonons at the Si/SiO2 interfaces results in a room temperature mobility much smaller than what is obtained using the common assumption of bulk phonons in the elastic, high-temperature approximation. We also find that, as a result of the complicated structure of the primed subbands, the high-field saturated velocity is significantly lower than its bulk value, as it had been measured in the past in the case of Si inversion layers but never explained theoretically. Finally, we find that IPP scattering does depress the low-field mobility but to a small extent, thanks to the presence of the interfacial SiO2 layers and to the proximity of the metal gates. Moreover, by keeping electrons `cooler', IPP scattering results in a higher saturated velocity. Therefore, the presence of high-kappa materials in the gate-insulator stacks should not affect negatively the performance of field effect transistors based on Si nanosheets.
△ Less
Submitted 15 August, 2026; v1 submitted 12 August, 2026;
originally announced August 2026.
-
Effects of phonon confinement on electron transport in Si nanowire and armchair-edge graphene nanoribbon transistors: A dissipative quantum-transport study
Authors:
Bimin Cai,
Maarten L. Van de Put,
Massimo V. Fischetti
Abstract:
Electronic transport in low-dimensional structures, such as thin bodies, nanosheets, nanoribbons and nanowires, is strongly affected by electron and phonon confinement, in addition to interface roughness. Here we use a quantum-transport formulation based on empirical pseudopotentials and the Master equation to study the effect of the phonon boundary conditions on the electron transport in field ef…
▽ More
Electronic transport in low-dimensional structures, such as thin bodies, nanosheets, nanoribbons and nanowires, is strongly affected by electron and phonon confinement, in addition to interface roughness. Here we use a quantum-transport formulation based on empirical pseudopotentials and the Master equation to study the effect of the phonon boundary conditions on the electron transport in field effect transistors (FETs) based on a small cross-section (3$\times$3 cells) Si nanowire (NW) and a 10 armchair graphene nanoribbon (10-aGNR). For the dispersion of the confined phonons we employ a simple empirical model based on the folding of the bulk phonon dispersion that approximates the results of the elastic-continuum model at long wavelengths. We consider two extreme cases for their boundary conditions: clamped boundary conditions (CBCs) or free-standing (FSBCs). We find that phonon confinement affects more severely the Si nanowires than graphene nanoribbons. In particular, for 3$\times$3 SiNW-FETs, CBCs result in a higher room-temperature electron mobility than FSBCs, a result consistent with what previously reported. On the contrary, in the off-equilibrium conditions seen in gate-all-around (GAA) 3$\times$3 SiNW-FETs with 7~nm gate-length, FSBCs yield a higher on-current than what is obtained assuming CBCs. However, for 10-aGNR-FETs, both the electron mobility and the on-current are higher when assuming FSBCs.
△ Less
Submitted 7 March, 2025;
originally announced March 2025.
-
Spatially Nonuniform Oscillations in Ferrimagnets Based on an Atomistic Model
Authors:
Xue Zhang,
Baofang Cai,
Jie Ren,
Zhengping Yuan,
Zhengde Xu,
Yumeng Yang,
Gengchiau Liang,
Zhifeng Zhu
Abstract:
The ferrimagnets, such as GdxFeCo(1-x), can produce ultrafast magnetic switching and oscillation due to the strong exchange field. The two-sublattices macrospin model has been widely used to explain the experimental results. However, it fails in describing the spatial nonuniform magnetic dynamics which gives rises to many important phenomenons such as the domain walls and skyrmions. Here we develo…
▽ More
The ferrimagnets, such as GdxFeCo(1-x), can produce ultrafast magnetic switching and oscillation due to the strong exchange field. The two-sublattices macrospin model has been widely used to explain the experimental results. However, it fails in describing the spatial nonuniform magnetic dynamics which gives rises to many important phenomenons such as the domain walls and skyrmions. Here we develop the two-dimensional atomistic model and provide a torque analysis method to study the ferrimagnetic oscillation. Under the spin-transfer torque, the magnetization oscillates in the exchange mode or the flipped exchange mode. When the Gd composition is increased, the exchange mode firstly disappears, and then appears again as the magnetization compensation point is reached. We show that these results can only be explained by analyzing the spatial distribution of magnetization and effective fields. In particular, when the sample is small, a spatial nonuniform oscillation is also observed in the square film. Our work reveals the importance of spatial magnetic distributions in understanding the ferrimagnetic dynamics. The method developed in this paper provides an important tool to gain a deeper understanding of ferrimagnets and antiferromagnets. The observed ultrafast dynamics can also stimulate the development of THz oscillators.
△ Less
Submitted 22 November, 2022;
originally announced November 2022.
-
Electric Field and Humidity Trigger Contact Electrification
Authors:
Yanzhen Zhang,
Thomas Pähtz,
Yonghong Liu,
Xiaolong Wang,
Rui Zhang,
Yang Shen,
Renjie Ji,
Baoping Cai
Abstract:
Here, we study the old problem of why identical insulators can charge one another on contact. We perform several experiments showing that, if driven by a preexisting electric field, charge is transferred between contacting insulators. This happens because the insulator surfaces adsorb small amounts of water from a humid atmosphere. We believe the electric field then separates positively from negat…
▽ More
Here, we study the old problem of why identical insulators can charge one another on contact. We perform several experiments showing that, if driven by a preexisting electric field, charge is transferred between contacting insulators. This happens because the insulator surfaces adsorb small amounts of water from a humid atmosphere. We believe the electric field then separates positively from negatively charged ions prevailing within the water, which we believe to be hydronium and hydroxide ions, such that at the point of contact, positive ions of one insulator neutralize negative ions of the other one, charging both of them. This mechanism can explain for the first time the observation made four decades ago that wind-blown sand discharges in sparks if and only if a thunderstorm is nearby.
△ Less
Submitted 14 January, 2015;
originally announced January 2015.
-
A possible mechanism for the negative capacitance observed in organic devices
Authors:
X. Q. Wang,
C. B. Cai
Abstract:
The mechanism of negative capacitance, e.g. inductance, induced by a sufficient electrical field in the organic device is investigated. The cations in organic bulk are proposed to be driven by the applied voltage and to accumulate at the interface, and further to generate the surface states or media states. These states result in a larger junction current through the device, indicating the negativ…
▽ More
The mechanism of negative capacitance, e.g. inductance, induced by a sufficient electrical field in the organic device is investigated. The cations in organic bulk are proposed to be driven by the applied voltage and to accumulate at the interface, and further to generate the surface states or media states. These states result in a larger junction current through the device, indicating the negative capacitances which are simulated in three situations: impedance spectrum, capacitance measurement and current response. This simple kinetic model may be helpful to understand why the negative capacitance phenomenon is observed in various organic devices.
△ Less
Submitted 20 November, 2012; v1 submitted 30 October, 2012;
originally announced October 2012.
-
Phototransistor Behavior Based on Dye-Sensitized Solar Cell
Authors:
X. Q. Wang,
C. B. Cai,
Y. F. Wang,
W. Q. Zhou,
Y. M. Lu,
Z. Y. Liu
Abstract:
In the present work, a light-controlled device cell is established based on the dye-sensitized solar cell using nanocrystalline TiO2 films. Voltage-current curves are characterized by three types of transport behaviors: linear increase, saturated plateau and breakdown-like increase, which are actually of the typical performances for a photo-gated transistor. Moreover, an asymmetric behavior is obs…
▽ More
In the present work, a light-controlled device cell is established based on the dye-sensitized solar cell using nanocrystalline TiO2 films. Voltage-current curves are characterized by three types of transport behaviors: linear increase, saturated plateau and breakdown-like increase, which are actually of the typical performances for a photo-gated transistor. Moreover, an asymmetric behavior is observed in the voltage-current loops, which is believed to arise from the difference in the effective photo-conducting areas. The photovoltaic voltage between the shared counter electrode and drain (VCE-D) is investigated as well, clarifying that the predominant dark process in source and the predominant photovoltaic process in drain are series connected, modifying the electric potential levels and thus resulting in the characteristic phototransistor behaviors.
△ Less
Submitted 24 October, 2012;
originally announced October 2012.
-
The electronic activity of boron and phosphorus impurities in a-Si and a-Si:H
Authors:
Bin Cai,
David A. Drabold
Abstract:
In amorphous materials, acceptor and donor impurities rarely dope the system (shift the Fermi level). We find out why in a-Si:H. We report simulations on B and P doping of a-Si:H and a-Si. We analyze the Electronic Density of States (EDOS) with concentrations ranging from 1.6% to 12.5% of B or P in a-Si. The results indicate that tetrahedral B and P are effective doping configurations in a-Si, but…
▽ More
In amorphous materials, acceptor and donor impurities rarely dope the system (shift the Fermi level). We find out why in a-Si:H. We report simulations on B and P doping of a-Si:H and a-Si. We analyze the Electronic Density of States (EDOS) with concentrations ranging from 1.6% to 12.5% of B or P in a-Si. The results indicate that tetrahedral B and P are effective doping configurations in a-Si, but high impurity concentrations introduce defect states. Clustered B or P also introduced mid-gap states. For a-Si:H, we report that both B(3,1) and P(3,1) (B or P atom bonded with three Si atoms and one H atom) are effective doping configurations. We investigate H passivation in both cases. There exists a "hydrogen poison range" for which H can modify the dopant configuration and suppress doping. For B doping, nearby H prefers to stay at the bond-center of Si-Si, leaves B four-fold and neutralizes the doping configuration; for P doping, nearby H spoils the doping by making tetrahedral P three-fold.
△ Less
Submitted 8 May, 2011;
originally announced May 2011.
-
Atomistic Simulations of Flash Memory Materials Based on Chalcogenide Glasses
Authors:
Bin Cai,
Binay Prasai,
D. A. Drabold
Abstract:
In this chapter, by using ab-initio molecular dynamics, we introduce the latest simulation results on two materials for flash memory devices: Ge2Sb2Te5 and Ge-Se-Cu-Ag. This chapter is a review of our previous work including some of our published figures and text in Cai et al. (2010) and Prasai & Drabold (2011) and also includes several new results.
In this chapter, by using ab-initio molecular dynamics, we introduce the latest simulation results on two materials for flash memory devices: Ge2Sb2Te5 and Ge-Se-Cu-Ag. This chapter is a review of our previous work including some of our published figures and text in Cai et al. (2010) and Prasai & Drabold (2011) and also includes several new results.
△ Less
Submitted 30 March, 2011;
originally announced March 2011.
-
The properties of amorphous GaN
Authors:
Bin Cai,
David A. Drabold
Abstract:
In this paper, we present three amorphous GaN models obtained from the first principles simulation. We find that a chemically ordered continuous random network is the ideal structure for a-GaN. If we exclude the tail states, we predict a 3.0eV optical gap for 64-atom model and 2.3eV for 250-atom models. We observe a highly localized valence tail and a remarkably delocalized exponential conduction…
▽ More
In this paper, we present three amorphous GaN models obtained from the first principles simulation. We find that a chemically ordered continuous random network is the ideal structure for a-GaN. If we exclude the tail states, we predict a 3.0eV optical gap for 64-atom model and 2.3eV for 250-atom models. We observe a highly localized valence tail and a remarkably delocalized exponential conduction tail which we associate with different hybridization in the two tails. Based upon these results, we speculate on potential differences in n and p type doping. The structural origin of tail and defect states is discussed. The vibrational density of states and dielectric function are computed, and are consistent with experiment.
△ Less
Submitted 8 March, 2011;
originally announced March 2011.