Kairolla S. Sekerbayev, Omid Farzadian, Azat Abdullaev, Yanwei Wang, Zhandos N. Utegulov
The effect of point defects (PDs) on interfacial thermal conductance (ITC) at the Si/3C–SiC interface is systematically investigated by nonequilibrium molecular dynamics simulations. Various PDs are introduced in the SiC interface region with atomic concentrations up to 5%. Our results show that carbon related vacancies significantly enhance ITC, with a linear increase observed as defect concentration rises. An amorphous SiC (a-SiC) interlayer is also modeled as a limiting case of defect-induced structural damage, resulting in a 35% increase in ITC compared to the pristine interface. Spectral decomposition and phonon-resolved analysis imply that defect-induced improvement in ITC takes place primarily due to low-frequency (below 10 THz) propagating phonons. The trade-off between improved heat transfer across the interface and reduced bulk thermal transport caused by defect-induced scattering is discussed. These findings provide valuable insight into phonon-mediated interfacial heat transport and demonstrate the potential of defect engineering strategies to improve interfacial thermal management in advanced SiC-based energy systems.
{"title":"Enhanced interfacial thermal conductance across Si/defected SiC interface","authors":"Kairolla S. Sekerbayev, Omid Farzadian, Azat Abdullaev, Yanwei Wang, Zhandos N. Utegulov","doi":"10.1063/5.0304881","DOIUrl":"https://doi.org/10.1063/5.0304881","url":null,"abstract":"The effect of point defects (PDs) on interfacial thermal conductance (ITC) at the Si/3C–SiC interface is systematically investigated by nonequilibrium molecular dynamics simulations. Various PDs are introduced in the SiC interface region with atomic concentrations up to 5%. Our results show that carbon related vacancies significantly enhance ITC, with a linear increase observed as defect concentration rises. An amorphous SiC (a-SiC) interlayer is also modeled as a limiting case of defect-induced structural damage, resulting in a 35% increase in ITC compared to the pristine interface. Spectral decomposition and phonon-resolved analysis imply that defect-induced improvement in ITC takes place primarily due to low-frequency (below 10 THz) propagating phonons. The trade-off between improved heat transfer across the interface and reduced bulk thermal transport caused by defect-induced scattering is discussed. These findings provide valuable insight into phonon-mediated interfacial heat transport and demonstrate the potential of defect engineering strategies to improve interfacial thermal management in advanced SiC-based energy systems.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"8 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rajat Bharadwaj, Parvathy Gireesan, Harikrishnan Sundaresan, Chithra H. Sharma, Lucky Donald L. Kynshi, Prasad Muragesh, D. Bougeard, Madhu Thalakulam
Solid-state quantum technologies such as quantum dot qubits and quantum electrical metrology circuits rely on ultra-low energy quantum phenomena, making them susceptible to various forms of environmental noise. Conventional passive filtering schemes can reduce high-frequency noise but are often ineffective against low-frequency interference, like powerline or instrument-induced. Extending such filters to lower frequencies causes issues such as longer stabilization times, slower system response, and increased Johnson noise, which impede low-frequency transport measurements. To address these limitations, we propose and experimentally demonstrate a generalized active noise cancelation scheme for quantum devices operating at sub-Kelvin temperatures. Our approach compensates periodic environmental interference by dynamically injecting a phase-coherent anti-noise signal directly into the device. We employ an automated feedback protocol featuring beat frequency reduction and adaptive phase-amplitude tuning, enabling real-time compensation without any manual intervention. Unlike post-processing or passive filtering, this method suppresses noise at the device level without introducing additional time constants. We implement the scheme on a gate-defined Si/SiGe quantum dot acting as a candidate system subject to strong 50 Hz powerline interference and validate its effectiveness through acquiring Coulomb blockade oscillations and Coulomb diamond plots. The technique achieves substantial suppression of both the targeted interference and the overall noise floor, thereby stabilizing transport characteristics and enhancing device fidelity. While demonstrated on a quantum dot, the proposed framework is broadly applicable to a wide class of solid-state quantum devices where deterministic noise presents a critical bottleneck. Our results establish active anti-noise injection as a versatile strategy for advancing noise-resilient quantum measurement platforms.
{"title":"Active noise reduction in gated quantum devices","authors":"Rajat Bharadwaj, Parvathy Gireesan, Harikrishnan Sundaresan, Chithra H. Sharma, Lucky Donald L. Kynshi, Prasad Muragesh, D. Bougeard, Madhu Thalakulam","doi":"10.1063/5.0303853","DOIUrl":"https://doi.org/10.1063/5.0303853","url":null,"abstract":"Solid-state quantum technologies such as quantum dot qubits and quantum electrical metrology circuits rely on ultra-low energy quantum phenomena, making them susceptible to various forms of environmental noise. Conventional passive filtering schemes can reduce high-frequency noise but are often ineffective against low-frequency interference, like powerline or instrument-induced. Extending such filters to lower frequencies causes issues such as longer stabilization times, slower system response, and increased Johnson noise, which impede low-frequency transport measurements. To address these limitations, we propose and experimentally demonstrate a generalized active noise cancelation scheme for quantum devices operating at sub-Kelvin temperatures. Our approach compensates periodic environmental interference by dynamically injecting a phase-coherent anti-noise signal directly into the device. We employ an automated feedback protocol featuring beat frequency reduction and adaptive phase-amplitude tuning, enabling real-time compensation without any manual intervention. Unlike post-processing or passive filtering, this method suppresses noise at the device level without introducing additional time constants. We implement the scheme on a gate-defined Si/SiGe quantum dot acting as a candidate system subject to strong 50 Hz powerline interference and validate its effectiveness through acquiring Coulomb blockade oscillations and Coulomb diamond plots. The technique achieves substantial suppression of both the targeted interference and the overall noise floor, thereby stabilizing transport characteristics and enhancing device fidelity. While demonstrated on a quantum dot, the proposed framework is broadly applicable to a wide class of solid-state quantum devices where deterministic noise presents a critical bottleneck. Our results establish active anti-noise injection as a versatile strategy for advancing noise-resilient quantum measurement platforms.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"34 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894039","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bismuthene, which is the Bi counterpart of graphene, is a promising candidate for the realization of a two-dimensional topological insulator that leads to the development of next-generation spintronic devices. In this study, we examined the atomic configuration of bismuthene grown on an Ag(111) surface at low temperatures using the total-reflection high-energy positron diffraction (TRHEPD) method. Pairs of TRHEPD rocking curves corresponding to the fractional-order spots of bismuthene islands exhibited no substantial differences in their profiles in the low-glancing-angle regions along the [112¯] and [11¯0] azimuths, confirming that bismuthene adopts a flat honeycomb lattice on the Ag(111) surface. Intensity calculations based on dynamical diffraction theory further revealed that the two Bi atoms in the unit cell have equivalent heights (2.48 Å) relative to the underlying Ag(111) layer. The Debye temperatures of bismuthene and Ag in the first layer are 92 and 112 K, respectively, indicating that both atoms experience softening. The structural insights obtained in this study provide a critical foundation for understanding the unique electronic properties of bismuthene and for designing applications in heterostructure devices.
{"title":"Atomic configuration of flat honeycomb lattice structure of bismuthene on Ag(111)","authors":"Yuki Fukaya, Iwao Matsuda","doi":"10.1063/5.0309407","DOIUrl":"https://doi.org/10.1063/5.0309407","url":null,"abstract":"Bismuthene, which is the Bi counterpart of graphene, is a promising candidate for the realization of a two-dimensional topological insulator that leads to the development of next-generation spintronic devices. In this study, we examined the atomic configuration of bismuthene grown on an Ag(111) surface at low temperatures using the total-reflection high-energy positron diffraction (TRHEPD) method. Pairs of TRHEPD rocking curves corresponding to the fractional-order spots of bismuthene islands exhibited no substantial differences in their profiles in the low-glancing-angle regions along the [112¯] and [11¯0] azimuths, confirming that bismuthene adopts a flat honeycomb lattice on the Ag(111) surface. Intensity calculations based on dynamical diffraction theory further revealed that the two Bi atoms in the unit cell have equivalent heights (2.48 Å) relative to the underlying Ag(111) layer. The Debye temperatures of bismuthene and Ag in the first layer are 92 and 112 K, respectively, indicating that both atoms experience softening. The structural insights obtained in this study provide a critical foundation for understanding the unique electronic properties of bismuthene and for designing applications in heterostructure devices.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"16 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894114","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shivangi Srivastava, Devendra K. Pandey, Divya P. Dubey, Anupam Bhattacharya, Ratnamala Chatterjee
We report the electrical and magneto-transport properties of [110]-oriented equiatomic GdPdBi thin films grown by pulsed laser deposition. Temperature-dependent resistivity measurements over the temperature range 3.5 K ≤ T ≤ 300 K indicate semiconducting behavior, with an activation energy gap of ∼10.2 meV, lower than the bulk bandgap (∼70 meV), suggesting strain-induced band narrowing in the thin films. Additionally, deviations from Nyquist behavior indicate electron–phonon scattering as the primary dephasing mechanism. A low-field cusp in the magneto-resistance, resembling weak anti-localization, is observed and attributed to three-dimensional bulk spin–orbit coupling, as confirmed by angle-dependent magneto-conductance measurements. The first-principles calculations confirm that a 1.2% biaxial strain reduces the bandgap from approximately 100 meV (unstrained) to 26 meV (strained), consistent with the experimental trend, and further indicate that the applied strain in GdPdBi induces the onset of band inversion. These findings provide insight into the transport properties and band structure of the GdPdBi half-Heusler thin films.
{"title":"Electrical and magneto-transport properties of GdPdBi half-Heusler thin films","authors":"Shivangi Srivastava, Devendra K. Pandey, Divya P. Dubey, Anupam Bhattacharya, Ratnamala Chatterjee","doi":"10.1063/5.0294505","DOIUrl":"https://doi.org/10.1063/5.0294505","url":null,"abstract":"We report the electrical and magneto-transport properties of [110]-oriented equiatomic GdPdBi thin films grown by pulsed laser deposition. Temperature-dependent resistivity measurements over the temperature range 3.5 K ≤ T ≤ 300 K indicate semiconducting behavior, with an activation energy gap of ∼10.2 meV, lower than the bulk bandgap (∼70 meV), suggesting strain-induced band narrowing in the thin films. Additionally, deviations from Nyquist behavior indicate electron–phonon scattering as the primary dephasing mechanism. A low-field cusp in the magneto-resistance, resembling weak anti-localization, is observed and attributed to three-dimensional bulk spin–orbit coupling, as confirmed by angle-dependent magneto-conductance measurements. The first-principles calculations confirm that a 1.2% biaxial strain reduces the bandgap from approximately 100 meV (unstrained) to 26 meV (strained), consistent with the experimental trend, and further indicate that the applied strain in GdPdBi induces the onset of band inversion. These findings provide insight into the transport properties and band structure of the GdPdBi half-Heusler thin films.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"21 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894038","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alexander Blackston, Alexandra Fonseca Montenegro, Sevim Polat Genlik, Maryam Ghazisaeidi, Roberto C. Myers
Recent ab initio calculations predict one-dimensional (1D) dispersive electronic bands confined to the atomic scale cores of dislocations in the wide bandgap (3.84 eV) semiconductor ZnS. We test these predictions by correlating sub-bandgap optical transitions with the density of dislocations formed during strain relaxation in epitaxial ZnS grown on GaP. The densities for four predicted partial dislocations are quantified using scanning electron microscopy-based electron channeling contrast imaging. Room-temperature ellipsometry reveals absorption peaks that scale with dislocation density and align with theoretical predictions. Low-temperature photoluminescence spectra show deep emission peaks matching dislocation 1D band-to-band transitions. Photoluminescence excitation spectroscopy reveals six distinct emission lines with contrasting excitation dependence. Four peaks (2.78, 2.41, 2.20, 1.88 eV), assigned to dislocations, exhibit only modest suppression (≤5×) when excited below the ZnS bandgap, while two other peaks (3.11, 1.53 eV) are strongly quenched (>10×). These findings support the existence of efficient, 1D band-to-band radiative transitions within quantum wire-like dislocation core states in ZnS, distinct from typical non-radiative deep level defects in wide gap semiconductors.
{"title":"Photoluminescence excitation spectroscopy of quantum wire-like dislocation states in ZnS","authors":"Alexander Blackston, Alexandra Fonseca Montenegro, Sevim Polat Genlik, Maryam Ghazisaeidi, Roberto C. Myers","doi":"10.1063/5.0301048","DOIUrl":"https://doi.org/10.1063/5.0301048","url":null,"abstract":"Recent ab initio calculations predict one-dimensional (1D) dispersive electronic bands confined to the atomic scale cores of dislocations in the wide bandgap (3.84 eV) semiconductor ZnS. We test these predictions by correlating sub-bandgap optical transitions with the density of dislocations formed during strain relaxation in epitaxial ZnS grown on GaP. The densities for four predicted partial dislocations are quantified using scanning electron microscopy-based electron channeling contrast imaging. Room-temperature ellipsometry reveals absorption peaks that scale with dislocation density and align with theoretical predictions. Low-temperature photoluminescence spectra show deep emission peaks matching dislocation 1D band-to-band transitions. Photoluminescence excitation spectroscopy reveals six distinct emission lines with contrasting excitation dependence. Four peaks (2.78, 2.41, 2.20, 1.88 eV), assigned to dislocations, exhibit only modest suppression (≤5×) when excited below the ZnS bandgap, while two other peaks (3.11, 1.53 eV) are strongly quenched (>10×). These findings support the existence of efficient, 1D band-to-band radiative transitions within quantum wire-like dislocation core states in ZnS, distinct from typical non-radiative deep level defects in wide gap semiconductors.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"386 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shuwei Tang, Guowei Wang, Shulin Bai, Pengfei Zhang, Peng Ai, Song Pei, Yilong Xiao, Yujie Bao, Zhanpeng Xu, Da Wan
Layered rare-earth oxides have become promising candidates for high-performance thermoelectric (TE) materials on account of the distinctive electronic structures and anisotropic transport properties. In this work, the phonon dynamics, carrier transport, and TE performance of the layered SmZnSbO compound are comprehensively evaluated using first-principles calculations, machine learning interatomic potentials, Boltzmann transport theory, and the two-channel model. The coexistence of weak interlayer van der Waals interactions, robust intralayer covalent bonding interactions, and rattling-like vibrations of Zn atoms synergistically induces significant lattice anharmonicity, resulting in a decreased lattice thermal conductivity (0.84 W/mK@900 K within the framework of the two-channel model) for the SmZnSbO compound. The natural quantum well architecture formed by the alternative conductive [Zn2Sb2]2− layer and the insulated [Sm2O2]2+ layer endows quasi-two-dimensional transport characteristics, enabling a high carrier mobility of 34.1 cm2/Vs. Moreover, the multi-valley electronic band structure with an indirect bandgap of 0.80 eV simultaneously optimizes electrical conductivity (σ) and Seebeck coefficient (S), resulting in an enhanced power factor. Benefiting from these synergistic features, the layered SmZnSbO compound achieves optimal dimensionless figures of merit (ZTs) of 1.47 and 1.40 for the p-type and n-type doping circumstances at 900 K. The current work not only elucidates the thermal and electronic transport mechanisms for the SmZnSbO compound but also establishes a paradigm for designing high-efficiency layered oxide TE materials through combined strategies of quantum confinement, phonon engineering, and multi-valley band convergence.
{"title":"Rattling-induced anharmonicity and multi-valley enhanced thermoelectric performance in layered SmZnSbO material","authors":"Shuwei Tang, Guowei Wang, Shulin Bai, Pengfei Zhang, Peng Ai, Song Pei, Yilong Xiao, Yujie Bao, Zhanpeng Xu, Da Wan","doi":"10.1063/5.0308503","DOIUrl":"https://doi.org/10.1063/5.0308503","url":null,"abstract":"Layered rare-earth oxides have become promising candidates for high-performance thermoelectric (TE) materials on account of the distinctive electronic structures and anisotropic transport properties. In this work, the phonon dynamics, carrier transport, and TE performance of the layered SmZnSbO compound are comprehensively evaluated using first-principles calculations, machine learning interatomic potentials, Boltzmann transport theory, and the two-channel model. The coexistence of weak interlayer van der Waals interactions, robust intralayer covalent bonding interactions, and rattling-like vibrations of Zn atoms synergistically induces significant lattice anharmonicity, resulting in a decreased lattice thermal conductivity (0.84 W/mK@900 K within the framework of the two-channel model) for the SmZnSbO compound. The natural quantum well architecture formed by the alternative conductive [Zn2Sb2]2− layer and the insulated [Sm2O2]2+ layer endows quasi-two-dimensional transport characteristics, enabling a high carrier mobility of 34.1 cm2/Vs. Moreover, the multi-valley electronic band structure with an indirect bandgap of 0.80 eV simultaneously optimizes electrical conductivity (σ) and Seebeck coefficient (S), resulting in an enhanced power factor. Benefiting from these synergistic features, the layered SmZnSbO compound achieves optimal dimensionless figures of merit (ZTs) of 1.47 and 1.40 for the p-type and n-type doping circumstances at 900 K. The current work not only elucidates the thermal and electronic transport mechanisms for the SmZnSbO compound but also establishes a paradigm for designing high-efficiency layered oxide TE materials through combined strategies of quantum confinement, phonon engineering, and multi-valley band convergence.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"21 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894023","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Optoelectronic logic gates, with high-speed, low-power consumption, and broad bandwidth, have attracted significant attention in high-density information processing applications. It would be more attractive and challenging to carry out multifunctional logic operations in an individual device due to the inherent nature of unidirectional carrier transport. Herein, a transistor-like one-dimensional ZnO/CH3NH3PbBr3 heterostructure is designed for an all-optically controlled logic gate that exhibits wavelength- and power-dependent bipolar photoresponse. Under visible light illumination, the device presents a negative photoresponse, while a transformation from negative to positive photoresponse emerges with increasing ultraviolet irradiation power. Time-resolved photoluminescence spectra demonstrate the carrier dynamics involving defect trapping about the negative-positive photoconductive switching. Based on the bipolar photoresponse, five fundamental logic operations (OR, AND, NOR, NOT, and NAND) are implemented in an individual device, which substantially enhances integration density while reducing power consumption. This work presents an optical sensing-computing integrated architecture for the multifunctional optoelectronic chips and non-Von Neumann intelligent sensors.
{"title":"All-optically controlled multifunctional logic gates based on the positive and negative photoresponse of a one-dimensional ZnO/CH3NH3PbBr3 heterostructure","authors":"Wendong Lu, Xiaoxuan Wang, Yi Ma, Wanyu Wang, Zhenhua Zhang, Wei Xia, Chaoyang Huang, Feifei Qin, Zengliang Shi, Chunxiang Xu","doi":"10.1063/5.0303564","DOIUrl":"https://doi.org/10.1063/5.0303564","url":null,"abstract":"Optoelectronic logic gates, with high-speed, low-power consumption, and broad bandwidth, have attracted significant attention in high-density information processing applications. It would be more attractive and challenging to carry out multifunctional logic operations in an individual device due to the inherent nature of unidirectional carrier transport. Herein, a transistor-like one-dimensional ZnO/CH3NH3PbBr3 heterostructure is designed for an all-optically controlled logic gate that exhibits wavelength- and power-dependent bipolar photoresponse. Under visible light illumination, the device presents a negative photoresponse, while a transformation from negative to positive photoresponse emerges with increasing ultraviolet irradiation power. Time-resolved photoluminescence spectra demonstrate the carrier dynamics involving defect trapping about the negative-positive photoconductive switching. Based on the bipolar photoresponse, five fundamental logic operations (OR, AND, NOR, NOT, and NAND) are implemented in an individual device, which substantially enhances integration density while reducing power consumption. This work presents an optical sensing-computing integrated architecture for the multifunctional optoelectronic chips and non-Von Neumann intelligent sensors.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"20 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bo Liu, Daguo Jiang, Yuxian Xie, Feng Lv, Haipeng Guo, Shenlin Zhou, Donglan Wu, Xianshi Zeng, Siqi Shi
Solid-state lithium metal batteries (SSLMBs) are promising for next-generation energy storage devices due to their superior energy density and excellent safety. Among solid-state electrolytes, garnet-type Li7La3Zr2O12 (LLZO) exhibits a wide electrochemical window and high lithium-ion conductivity, but poor electrode contact and Li dendrite growth restrict its practical application. To address these challenges, this study explores the application of thin film coatings composed of Li8MP4 (M = Si, Ge) at the lithium metal anode/LLZO interface. Through comprehensive first-principles thermodynamic calculations and hierarchical ion-transport algorithms, the phase stability, electrochemical stability, chemical stability, ionic transport, Li wettability, and mechanical properties of the candidate materials were systematically predicted and analyzed. Results indicate that the candidate coatings are thermodynamically stable at 0 K, with superior reduction stability against the lithium metal anode and good chemical compatibility with LLZO. Their Li-ion migration barriers are as low as 0.32 eV, enabling room-temperature ionic conductivity of approximately 10−5 S/cm. Moreover, the predicted works of adhesion for Li/Li8MP4 (M = Si, Ge) are 0.99 and 0.76 J/m2, respectively, corresponding to the contact angles of 0° and 49.3°, indicating that metallic Li shows good wettability on Li8MP4 (M = Si, Ge) materials. This work provides a comprehensive understanding of the thermodynamic and dynamic behaviors of Li8MP4 (M = Si, Ge) coatings and will guide the experimental design for desired SSLMB anode coatings.
{"title":"Predicting anode coatings for solid-state lithium metal batteries via first-principles thermodynamic calculations and hierarchical ion-transport algorithms","authors":"Bo Liu, Daguo Jiang, Yuxian Xie, Feng Lv, Haipeng Guo, Shenlin Zhou, Donglan Wu, Xianshi Zeng, Siqi Shi","doi":"10.1063/5.0307123","DOIUrl":"https://doi.org/10.1063/5.0307123","url":null,"abstract":"Solid-state lithium metal batteries (SSLMBs) are promising for next-generation energy storage devices due to their superior energy density and excellent safety. Among solid-state electrolytes, garnet-type Li7La3Zr2O12 (LLZO) exhibits a wide electrochemical window and high lithium-ion conductivity, but poor electrode contact and Li dendrite growth restrict its practical application. To address these challenges, this study explores the application of thin film coatings composed of Li8MP4 (M = Si, Ge) at the lithium metal anode/LLZO interface. Through comprehensive first-principles thermodynamic calculations and hierarchical ion-transport algorithms, the phase stability, electrochemical stability, chemical stability, ionic transport, Li wettability, and mechanical properties of the candidate materials were systematically predicted and analyzed. Results indicate that the candidate coatings are thermodynamically stable at 0 K, with superior reduction stability against the lithium metal anode and good chemical compatibility with LLZO. Their Li-ion migration barriers are as low as 0.32 eV, enabling room-temperature ionic conductivity of approximately 10−5 S/cm. Moreover, the predicted works of adhesion for Li/Li8MP4 (M = Si, Ge) are 0.99 and 0.76 J/m2, respectively, corresponding to the contact angles of 0° and 49.3°, indicating that metallic Li shows good wettability on Li8MP4 (M = Si, Ge) materials. This work provides a comprehensive understanding of the thermodynamic and dynamic behaviors of Li8MP4 (M = Si, Ge) coatings and will guide the experimental design for desired SSLMB anode coatings.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"129 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
InSe is a promising two-dimensional van der Waals semiconductor, exhibiting exceptional plasticity in its bulk single-crystalline form. This notable mechanical behavior originates from interlayer gliding and cross-layer dislocation slip, facilitated by the synergistic interplay between long-range In–Se Coulomb interactions spanning the van der Waals gap and soft intralayer In–Se bonding. To investigate anisotropic responses under strain, few-layer γ-InSe flakes on gold-coated transparent flexible PET substrates were subjected to ∼1.74% uniaxial tensile strain via substrate stretching, applied independently along both the armchair and zigzag crystallographic directions of γ-InSe. All Raman spectra of strained few-layer γ-InSe exhibit red shifts due to In–Se bond elongation, with distinct strain sensitivities observed across phonon modes [A1(Γ13) mode shows a shift rate of −0.6 cm−1/%, while the A1(Γ11), A1(Γ12), and E(Γ33) modes exhibit lower sensitivity at around −0.2 cm−1/%]. Under uniaxial strain, the absolute intensity of the dominant Raman peaks decreases significantly, whereas the relative intensity ratio of the emerging peaks at 147 and 155 cm−1 to the strongest peak (115 cm–1) shows a marked increase. Furthermore, angle-resolved polarized Raman spectroscopy (ARPRS) reveals a characteristic four-lobed pattern in the angular intensity distribution of γ-InSe, consistent with in-plane phonon anisotropy under C3v symmetry. This characteristic enables determination of the in-plane crystalline orientation through combined ARPRS measurements and group theory calculations. Our results demonstrate the suitability of the flexible substrate for such strain processes and establish Raman spectroscopy as an ultrasensitive method for strain determination in γ-InSe.
{"title":"Uniaxial strain-induced giant Raman enhancement in few-layer γ-InSe","authors":"Xiangnan Gong, Zhihao Wu, Chuanyao Yang","doi":"10.1063/5.0302001","DOIUrl":"https://doi.org/10.1063/5.0302001","url":null,"abstract":"InSe is a promising two-dimensional van der Waals semiconductor, exhibiting exceptional plasticity in its bulk single-crystalline form. This notable mechanical behavior originates from interlayer gliding and cross-layer dislocation slip, facilitated by the synergistic interplay between long-range In–Se Coulomb interactions spanning the van der Waals gap and soft intralayer In–Se bonding. To investigate anisotropic responses under strain, few-layer γ-InSe flakes on gold-coated transparent flexible PET substrates were subjected to ∼1.74% uniaxial tensile strain via substrate stretching, applied independently along both the armchair and zigzag crystallographic directions of γ-InSe. All Raman spectra of strained few-layer γ-InSe exhibit red shifts due to In–Se bond elongation, with distinct strain sensitivities observed across phonon modes [A1(Γ13) mode shows a shift rate of −0.6 cm−1/%, while the A1(Γ11), A1(Γ12), and E(Γ33) modes exhibit lower sensitivity at around −0.2 cm−1/%]. Under uniaxial strain, the absolute intensity of the dominant Raman peaks decreases significantly, whereas the relative intensity ratio of the emerging peaks at 147 and 155 cm−1 to the strongest peak (115 cm–1) shows a marked increase. Furthermore, angle-resolved polarized Raman spectroscopy (ARPRS) reveals a characteristic four-lobed pattern in the angular intensity distribution of γ-InSe, consistent with in-plane phonon anisotropy under C3v symmetry. This characteristic enables determination of the in-plane crystalline orientation through combined ARPRS measurements and group theory calculations. Our results demonstrate the suitability of the flexible substrate for such strain processes and establish Raman spectroscopy as an ultrasensitive method for strain determination in γ-InSe.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"72 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
It has been experimentally observed that Bi2O2Se—a semiconductor with nominally metallic conductivity—can undergo a metal–insulator transition (MIT), yet its microscopic origin remains unclear. Our hybrid density functional theory study uncovers the mechanism behind this transition. Under O- and Se-poor growth conditions, donor defects VO+ and VSe+ form at the highest concentrations, pushing the Fermi level above the conduction band minimum (CBM) and inducing metallic behavior in Bi2O2Se. As the chemical potentials of O and Se increase to moderate levels, the concentrations of VO+ and VSe+ drop, shifting the Fermi level down to the CBM and triggering the MIT. Further enrichment in O and Se yields only a weakly insulating phase, because the densities of VO2+ and VSe2+ rise unexpectedly under these rich conditions, preventing the emergence of a highly insulating phase. This counterintuitive trend is explained by defect-correlation mechanism.
{"title":"Microscopic origin of metal–insulator transition in two-dimensional Bi2O2Se unraveled by first-principles simulations","authors":"Chen-Min Dai, Feifan Bian, Chunlan Ma, Menglin Huang, Zenghua Cai, Shiyou Chen","doi":"10.1063/5.0311318","DOIUrl":"https://doi.org/10.1063/5.0311318","url":null,"abstract":"It has been experimentally observed that Bi2O2Se—a semiconductor with nominally metallic conductivity—can undergo a metal–insulator transition (MIT), yet its microscopic origin remains unclear. Our hybrid density functional theory study uncovers the mechanism behind this transition. Under O- and Se-poor growth conditions, donor defects VO+ and VSe+ form at the highest concentrations, pushing the Fermi level above the conduction band minimum (CBM) and inducing metallic behavior in Bi2O2Se. As the chemical potentials of O and Se increase to moderate levels, the concentrations of VO+ and VSe+ drop, shifting the Fermi level down to the CBM and triggering the MIT. Further enrichment in O and Se yields only a weakly insulating phase, because the densities of VO2+ and VSe2+ rise unexpectedly under these rich conditions, preventing the emergence of a highly insulating phase. This counterintuitive trend is explained by defect-correlation mechanism.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"30 1","pages":""},"PeriodicalIF":4.0,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145894040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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