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Squeezed Metallic Droplet with Tunable Kubo Gap and Charge Injection in Transition Metal Dichalcogenides

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Squeezed Metallic Droplet with Tunable Kubo Gap and Charge Injection in Transition Metal Dichalcogenides Squeezed metallic droplet with tunable Kubo gap and charge injection in transition metal dichalcogenides Jiaren Yuana,b,c, Yuanping Chena, Yuee Xiea, Xiaoyu Zhangb, Dewei Raob, Yandong Guod, Xiaohong Yana,b,1, Yuan Ping Fengc,e,1, and Yongqing Caif,1 aCollege of Science, Jiangsu University, 212013 Zhenjiang, China; bSchool of Material Science and Engineering, Jiangsu University, 212013 Zhenjiang, China; cDepartment of Physics, National University of Singapore, 117551 Singapore; dCollege of Electronic Science and Engineering, Nanjing University of Posts and Telecommunications, 210046 Nanjing, China; eCentre for Advanced Two-Dimensional Materials, National University of Singapore, 117551 Singapore; and fJoint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Taipa, Macau, China Edited by Donald G. Truhlar, University of Minnesota, Minneapolis, MN, and approved February 18, 2020 (received for review November 14, 2019) Shrinking the size of a bulk metal into nanoscale leads to the phases which trigger significant interests in catalysis and nano- discreteness of electronic energy levels, the so-called Kubo gap δ. electronics (13–16). Many of these TMDs, stabilizing in a hex- Renormalization of the electronic properties with a tunable and agonal (1H) phase, show a semiconducting characteristic with a size-dependent δ renders fascinating photon emission and electron strong spin–orbit coupling and excitonic effects, which are suitable tunneling. In contrast with usual three-dimensional (3D) metal clus- for diverse applications in field effect transistor (17), magnetic δ ters, here we demonstrate that Kubo gap canbeachievedwitha tunnel junction (18), valleytronics (19), and optoelectronic devices two-dimensional (2D) metallic transition metal dichalcogenide (i.e., (20). Unlike the 1H phase, the metallic octahedral 1T and its ′ 1T -phase MoTe2) nanocluster embedded in a semiconducting poly- distorted octahedral 1T′ phase exhibit a large magnetoresistance morph (i.e., 1H-phase MoTe ). Such a 1T′/1H MoTe nanodomain 2 2 (21), intriguing quantum spin Hall effect (22), and high catalytic resembles a 3D metallic droplet squeezed in a 2D space which activities (23, 24). Among the various TMDs, MoTe2 is particularly shows a strong polarization catastrophe while simultaneously main- ∼ taining its bond integrity, which is absent in traditional δ-gapped 3D interesting due to the smallest free energy difference [ 40 meV per clusters. The weak screening of the host 2D MoTe leads to photon unit cell (25, 26)] between the semiconducting 1H phase and me- 2 ′ emission of such pseudometallic systems and a ballistic injection of tallic 1T phase (27). Recent theoretical work revealed a laser- carriers in the 1T′/1H/1T′ homojunctions which may find applica- induced mechanism of vacancy ordering and growth of 1T′ seed CHEMISTRY tions in sensors and 2D reconfigurable devices. in the transition (28). By taking advantage of this phase tunability, here we demonstrate that through creating the 1T′/1H MoTe2 two-dimensional materials | Kubo gap | transition metal dichalcogenides coplanar heterophase structure, conducting carriers confined in 1T′ MoTe2 nanodomain show a Kubo gap opening. Different from the uantum confinement and surface effect strongly alter the traditional three-dimensional (3D) metallic nanoparticles which Qelectronic and chemical properties of nanoparticles ranging have undesirable surface dangling bonds, the conducting carriers in from atom to several nanometers (1). The electronic structure of the two-dimensional (2D) nanodomain which mimics a metallic a nanoparticle strikingly depends on the size. As the size of a droplet are squeezed into atomically thin 2D triangular space with metallic nanoparticle is reduced, its extending electronic wave- function becomes quantum-confined and electronic levels evolve Significance into shell-like behaviors, that is, discretization of energy levels (2). The average spacing of the successive levels, known as the We propose an approach to realize Kubo gap in 2D nanodomains, δ E N E N Kubo gap , scales with f/ , where f and are the Fermi which mimics three-dimensional (3D) metallic droplets squeezed energy of the bulk metal and the nuclearity of the particle, re- into atomically thin 2D space. We demonstrate 1H/1T′ phase spectively (3). For an Ag nanoparticle of 3 nm in diameter (N ∼ transition of the MoTe nanodomain driven by strain and excess 3 2 10 atoms) δ is 5 to 10 meV (4), while for an Na nanoparticle of carriers, and a strong anisotropy for a ballistic injection of carriers. 2.4 nm δ would be ∼26 meV (3). Striking phenomena occur when Breaking away from traditional trend of focusing almost exclu- δ is greater or comparable to thermal energy kBT (at room sively on 3D metal clusters for producing Kubo gap, our work temperature, kBT = 25 meV), which renders its nonmetallicity reveals the possibility of Kubo gap production in 2D systems like (5). The occurrence of the Kubo gap in metallic nanoparticles MoTe2. By overcoming the intrinsic limitations of the former, this also accounts for other fascinating properties such as signifi- approach can bring about potential technical possibilities, as well cantly lower melting points (6), nonmagnetic–magnetic transi- as new scientific activities related to the Kubo-gapped systems, tions (7), and changes in spectral features (8). However, the such as efficient quantum emitters and catalysis, and reconfig- moderate δ−gapped metallic particles tend to suffer from mul- urable devices. tiple structural variations, that is, isomerization of Ag and Au nanoparticles of different charging states (9, 10). The multiva- Author contributions: X.Y., Y.P.F., and Y. Cai designed research; J.Y. performed research; J.Y., Y. Chen, Y.X., X.Z., D.R., and Y.G. analyzed data; and J.Y., Y.P.F., and Y. Cai wrote lence of these nanoclusters leads to varying structures (11), un- the paper. stable magnetic ordering, and spin excitation (12), which severely The authors declare no competing interest. hinders their applications. Because of the dramatic structural discontinuity at the particle-vacuum/liquid interface of these This article is a PNAS Direct Submission. metallic nanoparticles it is hard to reach true monodispersity due Published under the PNAS license. to structural agglomerations and reconstruction. Data deposition: All files which were used to produce the data presented in this paper (atomic models of the transition metal dichalcogenides, input files, figures, etc.) have Here we demonstrate a scheme for the realization of a Kubo been deposited in the GitHub database at https://github.com/yuanjiaren/PNASdata. gap in a lattice-continual metallic nanophase embedded in a 1To whom correspondence may be addressed. Email: [email protected], [email protected]. semiconducting host using transition metal dichalcogenides sg, or [email protected]. (TMDs) MX2 (M: Mo or W and X: S, Se, or Te). These TMDs This article contains supporting information online at https://www.pnas.org/lookup/suppl/ have a strong lattice, spin, and orbital coupling and a wealth of doi:10.1073/pnas.1920036117/-/DCSupplemental. polymorphs with semiconducting (1H), metallic (1T and 1T′) www.pnas.org/cgi/doi/10.1073/pnas.1920036117 PNAS Latest Articles | 1of8 Downloaded by guest on September 25, 2021 well-passivated edge atoms. It is potentially useful for robust cre- phase diagram in the («, q) space is plotted through comparing ation/injection of quantum dots with a weak screening. the energies E (e, q) of the 1H and 1T′ phases, which are eval- uated by density functional theory (DFT) calculation, for each of Results the six group-VI TMDs. Reversible Phase Transition Induced by Charge Doping and Strain. Interestingly, all of the strain-doping curves corresponding to Group VI TMDs with the chemical formula MX2 (M: Mo or W the phase transition are monotonically U-shaped, indicating a and X: S, Se, or Te) have a variety of polymorph structures, such synergistic effect of the strain and carrier doping. The critical as the honeycomb 1H, 1T, and monoclinic 1T′ phases (Fig. 1 A– value of charge doping (strain) for driving the phase transition C) with space group of P6m2, P3m1, and P21/m, respectively. decreases when a uniaxial strain (charge doping) is applied si- The optimized lattice constants and the energetics relative to the multaneously. For instance, 0.13 q0 of electron doping or −0.2 q0 1H phase are given in SI Appendix, Table S1. The electronic of hole doping is required for the realization of the 1H–1T′ ′ structure and stability of 1H, 1T, and 1T MoTe2 are discussed in transition in MoTe2 without strain. With 3% strain, for both SI Appendix , Fig. S1. Governed by the crystal field-induced polarities only ∼0.05 q0 is required to activate the transition. Our splitting of the d-orbitals of the M cation, a facile transforma- findings explain the observed long-range phase transition of ′ tion from semiconducting 1H to metallic 1T/1T occurs, driven MoTe2 due to the charge transfer with a density of 0.11 q0 when 2 + – by increasing electron density of the M orbitals from d to the contacted with the 2D electride [Ca2N] ·e substrate (29). +x d2 via lithium exfoliation or doping. Since such a transition Concerning the pure strain effect without charge doping, our involves a strong orbital–lattice–charge coupling with breaking calculations reveal that only ∼4% strain is required to induce the octahedral symmetry of the 1H phase, below we mainly focus on 1H–1T′ phase transition of the MoTe2, which is consistent with the transition between the high symmetric 1H and the low the result of previous experiments (30). According to the ex- symmetric 1T′ phase. The estimation of the 1H–1T′ transition periment (30), a moderate tensile 0.2% strain can trigger the can serve as an upper limit for the metastable 1T phase in those transition at room temperature. This discrepancy between the 1H–1T and 1T–1T′ processes under external stress fields and experiment and our estimation may be due to the chemical ad- chemical doping.
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