Optoelectronic properties of high pressure regulated transition metal chalcogenides and their heterostructures

LI Chenkai; ZHU Jinlong

doi:10.7498/aps.74.20250498

Abstract

Semiconducting transition metal chalcogenides exhibit layer-dependent bandgaps, strong excitonic effects, and spin-valley coupling, positioning them as promising candidates for optoelectronic applications. In heterostructures formed by van der Waals stacking, interlayer excitons and moiré superlattices have emerged as a unique platform for exploring quantum many-body physics and correlated electronic phases. Subjecting semiconducting transition metal dichalcogenides and their heterostructures to high pressure enables precise, continuous tuning of optoelectronic properties through anisotropic lattice compression, particularly the dramatic reduction of interlayer distances, which greatly enhances interlayer orbital hybridization over traditional tuning methods. This review systematically presents diamond anvil cell techniques for in situ high-pressure characterization and analyzes the pressure-induced evolution in semiconducting transition metal dichalcogenides and their heterostructures. It focuses on four key aspects: 1) Atomic-scale structural phase transitions (e.g., layer sliding) and corresponding electronic band structure modifications, including direct-to-indirect bandgap transitions in monolayers (K-Λ crossover) and metallization/superconductivity; 2) Quantifiable enhancement of interlayer interactions revealed by layer-dependent phonon shifts and spin-orbit splitting amplification, along with the mechanisms of their influence on properties; 3) Modulation of exciton binding states and related mechanisms, covering intralayer excitons, trions and interlayer excitons; 4) Moiré potential modulation where high pressure significantly deepens potentials via interlayer compression. This review particularly highlights the unique capability of high pressure in enhancing interlayer orbital hybridization, thereby inducing exotic quantum phases. Finally, the future research directions in this field are outlined to advance quantum information device design, strongly correlated electron system simulation, and the novel excitonic state exploration.

Keywords:

Authors and contacts

LI Chenkai¹,
ZHU Jinlong^1,2,3

1.
Guangdong Basic Research Center of Excellence for Quantum Science, State Key Laboratory of Quantum Functional Materials, Department of Physics, Southern University of Science and Technology, Shenzhen 518055, China
2.
Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area (Guangdong), Shenzhen 518045, China
3.
Institute of Major Scientific Facilities for New Materials, Southern University of Science and Technology, Shenzhen 518055, China

Corresponding author: ZHU Jinlong, zhujl@sustech.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12274193, 12461160274), the Quantum Science Strategic Initiative of Guangdong Province, China (Grant No. GDZX2201001), the Basic Research Program of Shenzhen Natural Science Foundation, China (Grant No. K24205001), and the Major Science and Technology Infrastructure Program of Material Genome Big-science Facilities Platform supported by Municipal Development and Reform Commission of Shenzhen, China (Grant No. 2017-440300-82-01-293281/Historical Grant No. Z12017JY0012).

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Cited By

图 1 (a) 2H, 1T和1T'相单层TMD中原子结构示意图^[24]; (b) 已知的层状TMD的“周期表”, 根据所涉及的过渡金属元素进行组织, 总结了它们现有的结构, 并注明存在扭曲的结构和观察到的电子态^[24]; (c) 建立范德瓦耳斯异质结构的示意图^[27]

Figure 1. (a) Atomic structure of monolayer of TMDs in their trigonal prismatic (2H), distorted octahedral (1T) and dimerized (1T') phases^[24]; (b)“periodic table” of known layered TMDs, organized based on the transition metal element involved, summarizing their existing structural phases and indicating the presence of distorted structural phases and observed electronic phases^[24]; (c) schematic diagram of building van der Waals heterostructures^[27].

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图 2 (a) DAC横截面(左图)以及金刚石高压腔放大的示意图(右图) ^[40]; (b) 室温下红宝石在常压和2 GPa的荧光光谱^[54]; (c) 223—286 GPa的金刚石拉曼光谱, 上图纵轴为拉曼强度的一阶导数, 下图纵轴为拉曼强度, 上图中箭头指示拉曼峰的高频边缘, 定义为斜率最小处^[55]

Figure 2. (a) Schematic illustration of the cross-section of a DAC (left) , andthe zoom-in on the diamond/gasket assembly (right)^[40]; (b) illustration of the shift in position of the R1 fluorescence line of ruby on increasing pressure from ambient pressure to 2 GPa at room temperature^[54]; (c) (top) typical Raman spectra from the center of the diamond anvil culet at various pressures in 223–286 GPa range and (bottom) the differential spectrum at 286 GPa, the high-frequency edge of the Raman band was defined as a minimum of the differential^[55].

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图 3 (a) 2H_c和2H_a结构的MX₂的侧视图(投影在ac平面上)和俯视图(投影在ab平面上), M表示Mo或W, X表示S或Se, 红色箭头表示2H_c形成2H_a的层间滑移方向, 其中一个X-M-X单元(由蓝色框标记)在ab平面中移动^[66]; (b) 归一化的WSe₂晶格常数a/a₀, c/c₀和晶胞体积V随压力的演化^[64]; (c) 在压缩过程中, WSe₂的室温拉曼光谱^[64]; (d) WSe₂中A_1g和${\text{E}}_{{\text{2g}}}^{1} $模式峰位随压力的演化, 插图为A_1g和${\text{E}}_{{\text{2g}}}^{1} $模式振动示意图^[64]

Figure 3. (a) The side view (projected on ac plane) and top view (projected on ab plane) of 2H_c and 2H_a structure in MX₂, M represents Mo and W, X represents S and Se, the red arrows represent one sliding path for the 2H_c to 2H_a transition, where one unit of X-M-X triple layers (marked by a blue box) shifts in ab plane^[66]; (b) the normalized cell parameters a/a₀, c/c₀, and the volume V of WSe₂ as a function of pressure^[64]; (c) room temperature Raman spectra of WSe₂ in the compression^[64]; (d) peak frequencies of A_1g and ${\text{E}}_{{\text{2g}}}^{1} $ modes as a function of pressure of WSe₂, respectively, inset shows scheme of the Raman modes A_1g and ${\text{E}}_{{\text{2g}}}^{1} $^[64].

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图 4 (a) 少层和块体MoS₂的拉曼光谱^[67]; (b) $ {\text{E}}_{{\text{2g}}}^{1} $和A_1g拉曼模式的频率(左轴)及其差值(右轴)与层数的关系^[67]; (c) 不同层数N的MoS₂中A_1g和$ {\text{E}}_{{\text{2g}}}^{1} $模式随压强的演化, 插图为MoS₂的DCM模型^[72]; (d) 不同层数N中获得的$C_{\text{b}}^{\text{S}}/C_{\text{w}}^{\text{S}}$比值随压强的演化^[72]

Figure 4. (a) Raman spectra of thin and bulk MoS₂ films^[67]; (b) frequencies of $ {\text{E}}_{{\text{2g}}}^{1} $ and A_1g Raman modes (left vertical axis) and their difference (right vertical axis) as a function of layer thickness^[67]; (c) pressure-dependence of Raman shift of A_1g and $ {\text{E}}_{{\text{2g}}}^{1} $ with various N, and N changed from 2 to 9, and bulk, inset shows the DCM of MoS₂^[72]; (d) pressure-dependence of $C_{\text{b}}^{\text{S}}/C_{\text{w}}^{\text{S}}$ with various N^[72].

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图 5 (a) 层间呼吸模式和剪切模式示意图^[76]; (b) 衬底上的MCM模型^[72]; (c) 少层和块体MoS₂的斯托克斯和反斯托克斯拉曼散射光谱, 虚线和箭头用来指引特定拉曼峰^[72]; (d) 常压下MoS₂的拉曼峰位与层数N的关系^[72]; (e) MoS₂中的LB和S模式在高压下的蓝移速率与层数N的关系^[72]

Figure 5. (a) Schematics of interlayer breathing mode and shear mode^[76]; (b) MCM of MoS₂ on a solid substrate^[72]; (c) Stokes and anti-Stokes Raman spectra of the few-layer and bulk MoS₂ on a diamond surface, the dashed lines and arrows are used for guide^[72]; (d) Raman shifts of few-layer MoS₂ as a function of N^[72]; (e) N-dependence of Raman shifting rates of LB and S of MoS₂^[72].

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图 6 2H-MoS₂的压力-温度(P-T)相图^[79]

Figure 6. Pressure-temperature (P-T) phase diagram of 2H-MoS₂^[79].

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图 7 (a) 不同层数的少层MoS₂, WS₂, MoSe₂和WSe₂的能带结构图^[84]; (b) (上图)根据A峰强度归一化的MoS₂的PL光谱; (下图)单双层MoS₂的PL光谱, 插图为不同层数的PL量子产率^[19]

Figure 7. (a) Band structures of MoS₂, WS₂, MoSe₂, and WSe₂ with different thicknesses^[84]; (b) (top) normalized PL spectra by the intensity of peak A of thin layers of MoS₂; (bottom) PL spectra for mono- and bilayer MoS₂ samples. Inset: PL quantum yield in different layer^[19].

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图 8 计算得到的分别在(a) 0, (b) 2.1和(c) 2.5 GPa下的单层MoS₂的能带结构^[44]; (d) 基于计算的单层MoS₂带隙随压力的演化^[44]; (e) 单层TMD的能带结构和环境压力下单层MoS₂和WSe₂的双声子DRR过程的示意图, K-Q和K-K' 谷之间可能发生谷间散射, K-Q散射主要由M附近的声子介导, 而K-K' 散射涉及K附近的声子^[87]; (f) 高压下双层MoS₂样品的PL光谱图^[43]; (g) 双层MoS₂的PL峰位随压力的演化^[43]; (h) 当P = 0 GPa, 0 < P < 1.5 GPa和1.5 < P < 2.34 GPa时双层MoS₂能带结构的示意图^[43]

Figure 8. (a)–(c) Calculated band structures of monolayer MoS₂ at 0, 2.1, and 2.5 GPa, respectively^[44]; (d) functional relationships of bandgap versus pressure on monolayer MoS₂^[44]; (e) band structure of monolayer TMDs and schematic representation of the two-phonon DRR processes for monolayer MoS₂ and WSe₂ at ambient pressure, intervalley scattering between K-Q as well as K-K' valleys can occur, the K-Q scattering is mostly mediated by phonons near M, while K-K' scattering involves phonons near K^[87]; (f) PL spectra of the bilayer MoS₂ sample under high pressure^[43]; (g) photon energies of the PL peaks of the bilayer MoS₂ as a function of pressure^[43]; (h) schematic representations of the band structure for bilayer MoS₂ when P = 0 GPa, 0 GPa < P < 1.5 GPa, and 1.5 GPa < P < 2.34 GPa^[43].

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图 9 (a) 高压下单层MoSe₂的归一化差分反射光谱^[97]; (b) 在未压缩和压缩条件下, 单层MoSe₂在不同泵浦功率下的快、慢组分的荧光寿命τ₁和τ₂的平均值^[97]; (c) 高压-栅极电压调控的h-BN/MoSe₂/h-BN异质结器件的示意图^[98]; (d) 不同压力下单层MoSe₂的归一化PL光谱, 红色(蓝色)曲线表示栅极电压V_G = –3 V (3 V)^[98]; (e) 通过PL测量获得的单层MoSe₂的激子和三激子能量, 和三激子结合能$ E_{\text{b}}^{{\text{trion}}} $随压力的演化^[98]

Figure 9. (a) Normalized differential reflection signals under high pressure in monolayer MoSe₂^[97]; (b) the average values of fluorescence lifetime of two decay component τ₁ and τ₂ at different pump powers in monolayer MoSe₂ under uncompressed and compressed conditions^[97]; (c) schematic illustration of the high-pressure gating h-BN/MoSe₂/h-BN heterostructure setup^[98]; (d) normalized PL spectra of monolayer MoSe₂ under various pressures, the red (or blue) curve was obtained at V_G = –3 V (or 3 V)^[98]; (e) pressure-dependent exciton and trion states of MoSe₂ obtained by PL measurements and $ E_{\text{b}}^{{\text{trion}}} $ as a function of pressure^[98].

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图 10 (a) MoS₂/WS₂中$ {\text{A}}_{1}' $和$ {{\text{E}}'} $振动模式的拉曼峰位随压力的演化^[104]; (b) 转角为θ的垂直堆叠TMD示意图^[100]; (c) 层间间距和(d) 层间结合能与转角的关系, 以转角WS₂同质结为例^[100]; (e) 以转角MoS₂同质结为例, 模拟的5个在0°和60°下的高对称堆叠的拉曼光谱^[102]; (f) 3R和2H堆叠双层WS₂在0和17 GPa下的低频拉曼光谱^[107]; (g) 3R和2H堆叠双层WS₂中压力引起的层间压缩示意图^[107]

Figure 10. (a) Raman peak positions of the $ {\text{A}}_{1}' $ and $ {{\text{E}}'} $ vibration modes as a function of pressure on MoS₂/WS₂^[104]; (b) schematic diagram of vertically stacked TMD with a twist angle of θ^[100]; (c) the interlayer spacing, and (d) binding energy between two monolayers versus twist angles, as an example of WS₂^[100]; (e) simulated Raman spectra of the five high-symmetry stackings at 0° and 60°, as an example of twist bilayer MoS₂^[102]; (f) Raman spectra in 3R- and 2H-stacked bilayer WS₂ under 0 and 17 GPa.^[107]; (g) schematic of pressure induced interlayer compressing in 3R- and 2H-stacked bilayer WS₂^[107].

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图 11 (a) 单层MX₂^[112]、(b) MoS₂/WSe₂异质结^[115]和(c) MoS₂/WS₂异质结的能带示意图^[113]; (d) (上图)单层MoSe₂(黑线)、WS₂(粉线)和2°-MoSe₂/WS₂异质结(蓝线)的荧光光谱; (下图)MoSe₂/WS₂异质结中荧光峰峰位随转角的变化^[114]; (e) 不同转角的MoSe₂/WS₂异质结的归一化荧光光谱^[114]; (f)—(h) 计算的不同压力(0—2.8 GPa)下2H-WSe₂/MoSe₂异质结的能带结构^[111]

Figure 11. Band alignment for (a) MX₂ monolayers^[112], (b) MoS₂/WSe₂^[115] and (c) MoS₂/WS₂ heterostructures^[113]; (d) (top) PL spectra measured in MoSe₂ (black), WS₂ (pink) monolayers and MoSe₂/WS₂ heterostructure with a twist angle of 2° between the layers (blue); (bottom) Variation of the PL peak energy with twist angle in MoSe₂/WS₂; (e) normalized PL spectra in MoSe₂/WS₂ with interlayer twist angles ranging from 1° to 59°^[114]; (f)–(h) first-principles calculation results of electronic band structure of 2H-WSe₂/MoSe₂ heterostructures as a function of pressure in the 0–2.8 GPa range.^[111]

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图 12 (a) 随着层间相互作用强度的增大, Ⅱ型2D异质结中激子行为的演化^[111]; (b), (c) 高压下的归一化的WS₂/MoSe₂异质结的荧光光谱^[118]

Figure 12. (a) Evolution of the behavior of exciton in type-Ⅱ-alignment 2D heterostructures with increasing interlayer interaction strengths^[111]; (b), (c) normalized PL spectra on WS₂/MoSe₂ heterostructure under different pressures^[118].

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图 13 (a) (上图)R型MoSe₂/WSe₂异质结中的莫尔图案; (下图) 3个R型高对称点(A, B和C点)的侧视图和俯视图^[129]; (b) R型MoSe₂/WSe₂异质结中莫尔势与位置的关系^[129]; (c) 单层(绿色和橙色)的布里渊区和超晶格的mBZ的示意图^[29]; (d) 在mBZ中折叠的单层能带(绿色)的示意图, 莫尔势在mBZ边界处打开间隙, 产生平带(灰色)^[29]; (e) DFT计算的MoS₂在常压下沿Γ-M方向的声子色散谱, 垂直虚线表示莫尔矢量, 蓝色点表示常压下的拉曼光谱获得的莫尔声子M1, M2和M3的频率^[132]; (f) 归一化强度的莫尔声子强度与压强的关系^[132]; (g) 计算出的莫尔势深度和单层MoS₂带隙与压力的关系^[132]

Figure 13. (a) (Top) Moiré pattern in an R-type MoSe₂/WSe₂ heterostructure, (bottom) side-views and top-views of the three R-type local atomic registries (A, B, and C sites)^[129]; (b) the moiré potential of the interlayer exciton transition in an R-type MoSe₂/WSe₂ heterostructure^[129]; (c) schematic of the Brillouin zones of each monolayer (green and orange) and the mBZ of the superlattice^[29]; (d) schematic of monolayer bands (green) folded in the mBZ, the moiré potential opens a gap at the mBZ boundary, which produces flatter electronic bands (grey)^[29]; (e) DFT-calculated phonon dispersion of MoS₂ at ambient pressure along the Γ-M direction, the vertical dashed line indicates the moiré vector. The blue symbols represent the moiré phonon M1-, M2- and M3-peak frequencies obtained from the Raman spectra at ambient pressure^[132]; (f) pressure evolution of the normalized intensities of moiré phonons^[132]; (g) calculated moiré potential amplitude and MoS₂ bandgap in the heterostructure as functions of pressure^[132].

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