Formation, identification, and regulation mechanisms of interlayer excitons in TMD heterostructures

WANG Shuo; YIN Yao; WANG Lin

doi:10.7498/aps.74.20250890

Abstract
Interlayer excitons (IXs), formed in type-II van der Waals (vdW) heterostructures where electrons and holes reside in adjacent monolayers, have attracted increasing interest due to their spatially indirect nature, long lifetime, strong Coulomb binding, and unique out-of-plane dipole moment. These features make IXs a promising platform for exploring many-body physics and realizing next-generation excitonic devices. This review systematically presents the formation mechanisms, identification methods, and external modulation strategies of interlayer excitons in two-dimensional materials.First, we analye the prerequisites for the IX formation, emphasizing the role of band alignment, interlayer charge transfer, and momentum mismatch. Recent studies have also revealed that direct interlayer absorption is an alternative pathway for IX generatio. For identification, we summarize multiple optical techniques, including photoluminescence (PL), photoluminescence excitation (PLE), transient absorption (TA), and electro-absorption (EA). These techniques can detect IX energy positions, binding energies, and recombination pathways. However, distinguishing interlayer excitons from defect-bound or momentum-indirect excitons remains challenging in experiment due to spectral overlap and measurement-dependent explanation.Then, we review five primary external modulation methods: electric field, strain, magnetic field, twist angle, and optical cavities. Electric fields can realize fast, reversible tuning of exciton energy levels, especially for excitons with large dipole moments. Strain provides nanoscale spatial control and can reshape local potential landscapes. Magnetic fields affect the spin-valley configurations and allow access to exciton polarization dynamics. Moiré engineering via twist angles introduces periodic potential landscapes, yielding moiré-trapped IXs and novel hybrid exciton–polaritons. Optical cavities enhance exciton radiative recombination via light–matter coupling and open up possibilities for strong coupling regimes. We further discuss additional strategies such as substrate-induced screening, dielectric environment, probe-induced local stress, and ferroelectric gating, all of which enrich the modulation toolbox.To facilitate cross-comparison, we present a comprehensive summary table comparing different modulation approaches in terms of tuning targets, dimensionality, efficiency, dynamic responsiveness, and implementation complexity.Finally, we discuss emerging applications of IXs in optoelectronic and quantum devices. Their tunable emission and long-lived nature make them suitable for exciton-based memory, logic, lasers, and reconfigurable photonic circuits. With the development of material synthesis, interface engineering, and hybrid integration, interlayer excitons are evolving from basic quasiparticles to programmable excitonic elements in chip-scale photonics and quantum information technologies.

Keywords:
interlayer excitons /

van der Waals heterostructures /

exciton modulation /

spectroscopic identification
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图 1 TMD异质结构中层间激子的形成判定与多样化调控机制. 图中心展示典型异质结构中层间激子的空间构型及常用光谱学表征手段(PL, PLE, EA, TA), 外围示意常见调控方式, 包括电场、磁场、应力、光学微腔与扭转角等

Figure 1. Schematic of interlayer exciton identification and regulation. The center illustrates the spatial configuration of interlayer excitons and representative spectroscopic techniques (PL, PLE, EA, TA), surrounded by common external tuning approaches such as electric field, magnetic field, pressure, optical microcavity, and twist angle.

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图 2 层间激子的形成　(a) 单层WSe₂、单层MoSe₂和异质结构的光致发光光谱, 出自文献[19], 已获得授权; (b) 2D MoSe₂/WSe₂异质结的Ⅱ型半导体能带排列图, 出自文献[19], 已获得授权; (c) WSe₂/MoSe₂异质结及其单层组分的光致发光谱对比, 1.36 eV处的发光峰来源于层间激子复合, 出自文献[13], 已获得授权; (d) WSe₂/WS₂异质结构中层间激子的1s-2p跃迁(67 meV)中红外吸收谱, 出自文献[12], 已获得授权

Figure 2. Formation of interlayer excitons: (a) PL spectra of monolayer WSe₂, monolayer MoSe₂, and their heterostructure, reproduced with permission from Ref. [19]; (b) type-Ⅱ semiconductor band alignment diagram for the 2D MoSe₂/WSe₂ heterojunction, reproduced with permission from Ref. [19]; (c) comparison of PL spectra between the WSe₂/MoSe₂ heterojunction and its monolayer components, where the emission peak at 1.36 eV arises from interlayer exciton recombination, reproduced with permission from Ref. [13]; (d) mid-infrared absorption spectrum of the 1s-2p transition (67 meV) of interlayer excitons in the WSe₂/WS₂ heterostructure, reproduced with permission from Ref. [12].

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图 3 层间激子的判断　(a) 单层WS₂, MoS₂以及WS₂/MoS₂异质结构的PL谱, 出自文献[10], 已获得授权; (b) MoSe₂/WSe₂异质结构的PLE谱, 出自文献[50], 已获得授权; (c) 超快瞬态吸收(TA)谱中IXs形成的延迟(0.8 ps)与层间空穴转移(IHT)过程(0.2 ps), 出自文献[51], 已获得授权; (d) 电调制吸收(EA)谱中IX的本征吸收峰(1.359 eV, 1.377 eV)与PL间接跃迁峰(L1), 出自文献[37], 已获得授权

Figure 3. Identification of interlayer excitons: (a) PL spectra of monolayer WS₂, MoS₂, and the WS₂/MoS₂ heterostructure, reproduced with permission from Ref. [10]; (b) PLE spectrum of the MoSe₂/WSe₂ heterostructure, reproduced with permission from Ref. [50]; (c) formation dynamics of IXs (0.8 ps delay) and IHT (0.2 ps) observed in ultrafast TA spectroscopy, reproduced with permission from Ref. [51]; (d) intrinsic absorption peaks of IXs (1.359 eV, 1.377 eV) and indirect transition PL peak (L1) in EA spectroscopy, reproduced with permission from Ref. [37].

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图 4 电场调节层间激子密度　(a) WSe₂/MoSe₂激子晶体管结构示意图, 出自文献[31], 已获得授权; (b) 栅压调控激子流开关(ON/OFF状态)的PL强度对比, 出自文献[31], 已获得授权; (c) WSe₂/MoSe₂激子晶体管开关比随栅压的变化, 出自文献[31], 已获得授权; (d) 双栅极结构的WSe₂/MoSe₂异质结激子晶体管示意图, 出自文献[60], 已获得授权; (e) 无陷阱势与陷阱势下的层间激子光致发光空间分布图, 出自文献[60], 已获得授权; (f) 不同外栅电场下, 层间激子蓝移能量ΔE及对应的电子-空穴对密度随激发功率的变化关系, 出自文献[60], 已获得授权

Figure 4. Interlayer exciton density under electric field conditions: (a) Schematic of a WSe₂/MoSe₂ excitonic transistor structure, reproduced with permission from Ref. [31]; (b) comparison of PL intensities demonstrating exciton current switching (ON/OFF states) under gate voltage modulation, reproduced with permission from Ref. [31]; (c) gate voltage dependence of the ON/OFF ratio in WSe₂/MoSe₂ excitonic transistors, reproduced with permission from Ref. [31]; (d) schematic of a dual-gated WSe₂/MoSe₂ heterostructure excitonic transistor, reproduced with permission from Ref. [60]; (e) spatial distribution of interlayer exciton PL with and without trapping potentials, reproduced with permission from Ref. [60]; (f) electric-field-induced blue shift energy (ΔE) of interlayer excitons and corresponding electron-hole pair density as functions of excitation power under different external gate biases, reproduced with permission from Ref. [60].

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图 5 电场调控激子输运　(a) WSe₂/hBN/MoS₂三明治结构中激子扩散受电场势能(δE_el)与激子-激子排斥(δE_xx)协同调控的示意图, 出自文献[61], 已获得授权; (b) 激子传播距离L_x随静电势能与激子-激子排斥能比值δE_el/δE_xx的变化关系, 插图为模拟中的势能分布示意图, 出自文献[61], 已获得授权; (c) 纳米图案化MoSe₂/WSe₂异质结的器件示意图, 出自文献[62], 已获得授权; (d) MoSe₂/WSe₂异质结的三角形电势“滑道”设计示意图, 出自文献[62], 已获得授权; (e) 激发激光强度分布的CCD图像, 出自文献[62], 已获得授权

Figure 5. Electric-field-controlled exciton transport: (a) Schematic of exciton diffusion regulation in a WSe₂/hBN/MoS₂ sandwich structure through the synergistic effects of electric potential energy (δE_el) and exciton-exciton repulsion (δE_xx), reproduced with permission from Ref. [61]; (b) exciton propagation distance (L_x) as a function of the ratio between electrostatic potential energy and exciton-exciton repulsion energy (δE_el/δE_xx), with the inset showing the simulated potential energy distribution reproduced with permission from Ref. [61]; (c) device schematic of a nanopatterned MoSe₂/WSe₂ heterostructure reproduced with permission from Ref. [62]; (d) design schematic of triangular potential “channels” in a MoSe₂/WSe₂ heterostructure; (e) CCD image of the excitation laser intensity distribution reproduced with permission from Ref. [62].

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图 6 应变调控层间激子　(a) MoS₂/WSe₂异质双层中周期性褶皱结构的示意图, 波峰与波谷分别引入拉伸与压缩应变, 出自文献[69], 已获得授权; (b) 激子发射峰值能量随皱褶轮廓的连续移动, 总调节范围达107 meV, 出自文献[69], 已获得授权; (c) MoSe₂/WSe₂异质结构中双轴应变下层间和层内激子结合能的GW+BSE计算结果, 出自文献[70], 已获得授权; (d), (e) WSe₂/WS₂异质结构在拉伸应变下PL增强及谷极化效应(10 K下极化度达20%), 出自文献[71], 已获得授权; (f) 应变诱导的谷间不等势示意图, 出自文献[71], 已获得授权; (g) WSe₂/MoSe₂异质结构在静水压力下激子态演化过程及能带重排示意图, 出自文献[65], 已获得授权; (h), (i) 静水压力诱导的能带重排示意图(低压与高压下的能带对齐变化), 出自文献[65], 已获得授权

Figure 6. Strain-engineered interlayer excitons: (a) Schematic of periodic wrinkle structures in MoS₂/WSe₂ heterobilayers, where peak and valley regions introduce tensile and compressive strains, respectively, reproduced with permission from Ref. [69]; (b) continuous tuning of exciton emission peak energy along the wrinkle profile, showing a total modulation range of 107 meV, reproduced with permission from Ref. [69]; (c) GW+BSE calculated binding energies of interlayer and intralayer excitons under biaxial strain in MoSe₂/WSe₂ heterostructures, reproduced with permission from Ref. [70]; (d), (e) PL enhancement and valley polarization effects (20% polarization degree at 10 K) in WSe₂/WS₂ heterostructures under tensile strain, reproduced with permission from Ref. [71]; (f) schematic of strain-induced valley potential inequality, reproduced with permission from Ref. [71]; (g) evolution of excitonic states and band rearrangement in WSe₂/MoSe₂ heterostructures under hydrostatic pressure, reproduced with permission from Ref. [65]; (h), (i) schematic of pressure-induced band rearrangement (low-pressure vs. high-pressure band alignment), reproduced with permission from Ref. [65].

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图 7 磁场调控层间激子　(a) WSe₂/MoSe₂异质结构中自旋单重态(IX_S)与三重态(IX_T)的PL谱随磁场的变化, 出自文献[27], 已获得授权; (b) IX_S和IX_T的谷Zeeman劈裂能隙及g因子(高达~15.2)的磁场依赖关系, 出自文献[27], 已获得授权; (c), (d) H型和R型堆叠异质结在24.2 T磁场下的谷极化度共振增强现象, 出自文献[80], 已获得授权; (e) WSe₂/YIG异质结构中中性激子(X₀)和带电激子(T)的谷极化度随磁场的变化, 出自文献[82], 已获得授权; (f) 谷塞曼劈裂随外磁场的线性变化特征, 出自文献[82], 已获得授权

Figure 7. Magnetic-field-controlled interlayer excitons: (a) Magnetic-field-dependent PL spectra of spin-singlet (IX_S) and triplet (IX_T) states in WSe₂/MoSe₂ heterostructures, reproduced with permission from Ref. [27]; (b) valley Zeeman splitting energy gaps and magnetic-field dependence of g-factors (up to ~15.2) for IX_S and IX_T states, reproduced with permission from Ref. [27]; (c), (d) resonance-enhanced valley degree of polarization (DOP) in H-type and R-type stacked heterostructures under 24.2 T magnetic field, Reproduced with permission from Ref. [80]; (e) magnetic-field evolution of valley polarization for neutral excitons (X₀) and charged excitons (T) in WSe₂/YIG heterostructures, reproduced with permission from Ref. [82]; (f) linear dependence of valley Zeeman splitting on external magnetic field, reproduced with permission from Ref. [82].

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图 8 扭转角调控层间激子　(a) WS₂/WSe₂异质结构中ADF-STEM成像显示的~7.6 nm莫尔周期, 出自文献[5], 已获得授权; (b), (c) WSe₂/WS₂异质结构中激子PL强度及跃迁路径(K-K直接跃迁与Q-K间接跃迁)随扭转角的变化, 出自文献[87], 已获得授权; (d), (e) 不同扭转角下层间激子圆偏振发射方向反转及极化度周期性波动行为, 出自文献[88], 已获得授权; (f) MoSe₂/WSe₂异质结构中层间激子寿命随扭转角的变化趋势(1°—3.5°), 出自文献[90], 已获得授权

Figure 8. Twist-angle-engineered interlayer excitons: (a) ADF-STEM image of a WS₂/WSe₂ heterostructure showing moiré superlattices with ~7.6 nm periodicity, Reproduced with permission from Ref. [5]; (b), (c) twist-angle dependence of excitonic PL intensity and transition pathways (direct K-K transition vs. indirect Q-K transition) in WSe₂/WS₂ heterostructures, reproduced with permission from Ref. [87]; (d), (e) circularly polarized emission reversal and periodic oscillations of polarization degree under different twist angles, reproduced with permission from Ref. [88]; (f) interlayer exciton lifetime evolution with twist angle (1° to 3.5°) in MoSe₂/WSe₂ heterostructures, reproduced with permission from Ref. [90].

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图 9 光场共振调控　(a) 4.2 K下的腔装置, 基于光纤的微镜与顶部带有化学气相沉积(CVD)生长的MoSe₂-WSe₂异质结构的平面宏观镜共同构成腔体, 出自文献[92], 已获得授权; (b) 器件结构示意图, 包含一个被hBN包裹的MoSe₂/WSe₂异质双层, 上下层均有石墨烯(Gr)层. 底部栅极电压(V_BG)和顶部栅极电压(V_TG)分别施加在石墨烯层上, 而TMD薄片接地(GND), 该腔体由底部和顶部的SiO₂层以及范德瓦耳斯异质堆叠组成, 出自文献[93], 已获得授权; (c) 层间激子(IX)的总积分光致发光(PL)强度(红色)和寿命(蓝色)随电场E_z的变化关系, 出自文献[93], 已获得授权; (d) 右列为无PLoM结构(上)和有PLoM结构(下)的异质结示意图, 左列为无PLoM结构(上)与有PLoM结构(下)层间激子光致发光的映射图像, 出自文献[94], 已获得授权; (e) 不同绝缘层(hBN, 红色; SiO₂, 蓝色)情况下, 拉比分裂随层数平方根的变化关系. 可以发现耦合强度存在明显的N^1/2(层数的平方根)增强效应, 出自文献[96], 已获得授权; (f) 上图为不同泵浦密度下零失谐时莫尔下极化激元(LPs)和中极化激元(MPs)的反射光谱, 下图为莫尔异质双层极化激元能量位移与载流子密度的关系, 出自文献[98], 已获得授权

Figure 9. Optical field resonance control: (a) Cavity setup at 4.2 K, the fiber-based micro-mirror forms the cavity together with a planar macro-mirror with CVD-grown MoSe₂-WSe₂ heterostructure on top, reproduced with permission from Ref. [92]; (b) schematic of the device structure, comprising a MoSe₂ /WSe₂ heterobilayer encapsulated with hBN, with bottom and top graphene (Gr) layers, bottom (V_BG) and top (V_TG) gate voltages are applied to the graphene layers, respectively, while the TMD flakes are grounded (GND), the cavity consists of the bottom and top SiO₂ layers and the van der Waals heterostack, reproduced with permission from Ref. [93]; (c) total integrated IX PL intensity (red) and lifetime (blue) as a function of E_z, reproduced with permission from Ref. [93]; (d) the right column shows the schematic diagrams of the heterojunction without PLoM structure (top) and with PLoM structure (bottom), while the left column presents the photoluminescence mapping images of interlayer excitons without PLoM structure (top) and with PLoM structure (bottom), reproduced with permission from Ref. [94]; (e) Rabi splitting as a function of the square root of the number of layers for different insulators, hBN (red) and SiO₂ (blue), a clear N^1/2 enhancement of the coupling strength is found, reproduced with permission from Ref. [96]; (f) the upper figure shows the reflection spectra of moiré lower polaritons (LPs) and middle polaritons (MPs) at zero detuning under different pumping densities, the lower figure shows the relationship between the energy shift of moiré heterobilayer polaritons and carrier density, reproduced with permission from Ref. [98].

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图 10 其他调控手段　(a), (b) WSe₂/MoSe₂异质结构中自旋单态(IX_singlet)与三重态(IX_triplet)的PL强度随温度的变化, 出自文献[99], 已获得授权; (c) 三层WSe₂/WSe₂/MoSe₂异质结构中双WSe₂夹层构型对激子发光强度的增强效应(近20倍), 出自文献[102], 已获得授权

Figure 10. Additional modulation approaches: (a), (b) Temperature-dependent PL intensity evolution of spin-singlet (IX_singlet) and triplet (IX_triplet) states in WSe₂/MoSe₂ heterostructures, reproduced with permission from Ref. [99]; (c) dual-WSe₂ sandwich configuration in WSe₂/WSe₂/MoSe₂ trilayer heterostructures showing near 20× exciton emission enhancement, reproduced with permission from Ref. [102].

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表 1 层间激子的主要调控手段对比

Table 1. Comparison of main regulation methods for interlayer excitons.

调控手段	主要调控对象	调控维度	调控效率/范围	动态响应性	空间分辨率	实验难度	典型应用
电场	能级漂移^{[31,56,60,62,64,105]} 偶极矩调制^[55,57]	能量强度	可达数十^{[56,58,60,64]}~百^[62] meV	高	中	中	能带调控^[55,62,64]发光增强^[106]
应变	能带结构^{[64,66–69,72,73]}结合能^[65]谷分裂^[74]	能量极化度	可达百 meV^[65,69], 结合能下降^[65]	中–低	高	中	态重构^{[68,69,72–74]}波导设计^[67]
磁场	自旋/谷态分裂态简并破缺^[27,80–83]	能级极化度	~meV 级^{[18,27,34,75,77,80]}	高	低	高	谷电子学^{[16,18,27,75,76,80]}拓扑探索^[34,77]
扭转角	态耦合^[25,85,87]moire 调制^{[5,54,84,86,88,89]}	能带极化态	可诱导新态生成^{[25,54,84–86,89,90]}	固定	中	高	极化子^[25,87,88]束缚态调控^{[5,54,84–86,89]}
光场	辐射效率^[92–94,96] 发射模式^[95,97,98]	发光强度寿命	可增强数十倍^[93,94,96]	高	高	中–高	强耦合^[92,96–98]PL增强^[93–95]
其他	双激子转化局域势场扰动等	能量、态密度	不等(视手段)	高-低	高	中	探针调控^[101]热场诱导^[83,104]

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