Abstract
Tunnel nanojunctions based on inelastic electron tunneling (IET) have been heralded as a breakthrough for ultra-fast integrated light sources. However, the majority of electrons tend to tunnel through a junction elastically, resulting in weak photon-emission power and limited efficiency, which have hindered their practical applications to date. Resonant tunneling has been proposed as a way to alleviate this limitation, but photon-emissions under resonant tunneling conditions have remained unsatisfactory for practical IET-based light sources due to the inherent contradiction between high photon-emission efficiency and power. In this work, we introduce a novel approach that leverages much stronger resonant tunneling enhancement achieved by multiple metallic quantum wells, which has enabled the internal quantum efficiency to reach ∼1 and photon-emission power to reach ∼0.8 µW/µm2. Furthermore, this method is applicable with different electronic lifetimes ranging from 10 fs to 100 fs simultaneously, bringing practical implementation of IET-based sources one step closer to reality.
1 Introduction
As the essential components of optoelectronic devices, the quest for an ideal photon source that can emit photons with ultra-fast speed, high efficiency, and sufficient power in miniaturized scale is a critical research focus [1–3]. Among the various light sources, the tunnel junctions based on inelastic electron tunneling (IET) events have gained extensive attention for their unique potential to provide ultra-compact sources with unprecedented photon modulation speed exceeding THz [4–7]. This fast photon-emission speed is attributed to the extremely short tunneling time (<10 fs) [8–10]. However, the low photon-emission efficiency (internal quantum efficiency, IQE <10 %) and radiation power (P r ∼ pW/µm2) have severely restricted their practical applications to date. Therefore, comprehensive investigation of the fundamental mechanisms to improve the IQE and P r , and the interrelation between the IQE and P r is imperative.
Figure 1(a) depicts a typical metal–insulator–metal (MIM) tunnel junctions with a biased field. The quantum tunneling mechanism enables electrons to tunnel across barriers elastically or inelastically, forming a tunneling current, even if their energy is lower than the potential energy of the barriers. Elastic tunneling (ET) means electrons have no energy loss during the tunneling process (as shown in the process 1). In contrast, inelastic tunneling events (as depicted in process 2) involve electrons losing energy while tunneling, leading to photon emission [4, 11, 12]. This photon generation process can be described as a two-step process [13]: First, surface plasmons are excited by the inelastic tunneling electrons. The ratio between inelastic (Γ
ie
) and elastic (Γ
e
) tunneling rate is defined as

The schematic diagram of MIM, single MQW and mMQW systems. (a) The structure of classical tunnel-junctions based sources and corresponding potential energy diagram with biased field. Process (1) represents the ET events and process (2) represents the IET events. One can see clearly the opposite trend of IQE and Γ ie , indicating the contradiction between high-IQE and large-P r . (b) The resonance-built system formed by single MQW. By bridging one resonant tunneling channel, electrons will have higher probability across the barrier. Note that the resonant electron tunneling rate increases faster than the non-resonant electron tunneling rate. (c) The RIET-built light generation unit. By taking advantage of RIET enhancement factor utilizing 3-MWQs system, simultaneous improvement of high-IQE and large-P r is possible without the unessential restrictions. Note that when the barrier thickness approaches zero, the tunneling events would become negligible.
Hence, a crucial aspect for the realization of optimal IET light sources is to engineer a structure that can facilitate a more rapid increase of Γ
ie
as compared to the Γ
e
. A commonly adopted approach is to improve the optical properties of the structure by enhancing the local density of optical states (LDOS) [13, 14, 16, 17]. The enhancement of LDOS enables larger Γ
ie
with minimal impacts on Γ
e
, leading to simultaneous growth of IQE and P
r
. However, this method will break down when the electric-field intensity is strong enough [18], limiting the maximum achievable IQE (<50 %) [17]. Moreover, the LDOS-enhancement is highly dependent on the design of intricate nanostructures, requiring complex fabrication processes. Therefore, an inevitable strategy is to engineer the tunneling rate from an additional point of view: The electrical properties through the resonance effect. When the energy of tunneling electrons matches one of the discrete energy levels formed by a quantum well (QW), the tunneling transmission coefficient can be greatly enhanced via resonant electron tunneling. More importantly, this approach demonstrates the faster increase of resonant electron tunneling rate (Γres) in comparison to the non-resonant electron tunneling rate (Γnon-res). Consequently, the resonant enhancement (
In this work, we have addressed the challenge of improving RIET enhancement by exploring the multiple metallic quantum wells (mMQWs) structures. More specifically, our study demonstrates that the tunneling transmittance in 3-MQWs resonance case is 6 orders of magnitude larger than the cases in non-resonant tunneling condition. By utilizing 3-MQWs resonance system in the tunnel junctions, we resolve the inconsistency between high-IQE and large-P r (the darkest red cure in the Figure 1(c)), realizing the IQE ∼ 1 and P r ∼ 0.8 µW/µm2 in the best cases, with an electron lifetime ranging from 10 fs to 100 fs. The proposed mMQWs-based approach offers a promising pathway to overcome the limitations of traditional IET-based photon sources and provides a viable platform for the development of ultra-fast and high-efficiency optoelectronic devices.
2 Results and discussion
2.1 The mismatch between high-IQE and large-P r in MIM tunneling junctions and single MQW system
In the framework of the transfer-Hamiltonian formalism [21], both the Γ
e
and Γ
ie
can be introduced via perturbation theory and Fermi’s golden rule. Then, the relationship between IQE and P
r
can be investigated from the simplest case: MIM tunnel junction. Here, we choose TiN as the bottom electrode/metallic layer of MQW while Al2O3 served as the insulating layer based on the lattice matching between TiN and Al2O3, which aids in the growth of single crystal Al2O3 and avoid leakage current caused by dielectric defect states. In addition, ITO is chosen as the top electrode due to its high transparency and efficient photon radiation properties. Figure 2(a) shows the potential energy of the typical MIM tunnel junction and corresponding wave functions of the left/right electrodes (φ
ν/μ
). In the barrier regime with thickness b, the φ
ν/μ
decay exponentially with distance from the respective electrode, which are described as φ
ν
(z) = φ
ν
e
−Kz
and
![Figure 2:
The features of IET rate with resonant enhancement brought from single MQW. (a) The potential energy and corresponding wavefunctions diagram of MIM tunneling junctions. (b) The
Γ
i
e
Γ
e
$\frac{{{\Gamma }}_{ie}}{{{\Gamma }}_{e}}$
(black line) and normalized P
r
(red line) distribution with barrier thickness which presents completely conversed trends with respect to barrier thickness. (c) The potential energy and wavefunctions of single MQW with RIET establishment. (d) The EΓ curves under different barrier thickness cases. The obvious peaks indicate the establishment of resonant tunneling. (e–f) The variation of
Γ
r
_
i
e
Γ
n
_
e
$\frac{{{\Gamma }}_{r\text{\_}ie}}{{{\Gamma }}_{n\text{\_}e}}$
with total bias voltage (V) drop across the tunnel junctions. Considering that two potential barriers play distinguishable roles in the electron tunneling process, we analyze the variation of
Γ
r
_
i
e
Γ
n
_
e
(
b
1
,
b
2
)
$\frac{{{\Gamma }}_{r\text{\_}ie}}{{{\Gamma }}_{n\text{\_}e}}({b}_{1},{b}_{2})$
with each barrier thickness b
1 (e) and b
2 (f), respectively. One can note that
Γ
r
_
i
e
Γ
n
_
e
(
V
)
$\frac{{{\Gamma }}_{r\text{\_}ie}}{{{\Gamma }}_{n\text{\_}e}}(V)$
curves form the obvious peaks, indicating the realization of RIET-enhanced IQE when precise resonant condition of V is achieved. In addition, negative-slope of
Γ
r
_
i
e
Γ
n
_
e
b
2
$\frac{{{\Gamma }}_{r\text{\_}ie}}{{{\Gamma }}_{n\text{\_}e}}\left({b}_{2}\right)$
does not mean that b
2 = 0 nm is the best case. Because the establishment of resonant cavity formed by double barriers is the premise of this numerical simulation [23, 24].](/document/doi/10.1515/nanoph-2023-0231/asset/graphic/j_nanoph-2023-0231_fig_002.jpg)
The features of IET rate with resonant enhancement brought from single MQW. (a) The potential energy and corresponding wavefunctions diagram of MIM tunneling junctions. (b) The
Here, E is the incident energy of electron, ρ
ν/μ
are the electronic density of states for the left/right electrons, Z
0is an arbitrary point in the barrier region,
Based on the derived formula of P
r
and
A more sophisticated tunnel junction system is proposed to increase the IQE by engineering the electrical properties using RIET effect. In such RIET-built system, the potential energy and confined wave function of a double barrier structure with a QW placed between the barriers is shown in Figure 2(c). Note that, regarding the working wavelengths of IET-sources in visible and near-infrared regimes, metallic quantum wells (MQWs) are commonly utilized because they have deeper potential well and support emitting higher-energy photon compared with the semiconductor quantum wells. When the incident energy of electron matches the discrete energy level formed by the MQW, a resonant tunneling phenomenon occurs. The resonant tunneling induces a large transmission coefficient attributed to the constructive interference between the wavefunctions transmitted and reflected from the barriers [22]. Therefore, adding resonant tunneling channels to IET events while non-resonant paths for the ET transmission is an effective strategy to enhance the IQE [13]. Considering the RIET system built by a MIMIM tunneling structure with well width of a and the surrounding barriers width as b 1 and b 2, the function of resonant IET rate(Γ r_ie ) and non-resonant ET rate (Γ n_e ) are found to be (see details in Supplementary Material Section 4):
Here, Γ is original tunneling transmission coefficients which is calculated by piece-wise linear approximation method.
Then the
2.2 The elimination of contradictions in mMQWs system
A straightforward next step is to further improve the effect of resonant enhancement and reverse the trend of
![Figure 3:
The breakdown of contraction between high-IQE and large P
r
by mMQW systems. (a) The potential energy and corresponding wavefunctions of mMQWs system. (b) The EVΓ map of the engineered mMQWs system. (c) The EΓ curves under resonant voltages with different c
2. It is worth to note that, by considering the practical fabrication with certain thickness variation, such RIET enhancement from mMQWs may give a relatively lower value (see detailed discussion in Supplementary Material Section 10). (d–e) The variation of
Γ
r
_
i
e
Γ
n
_
e
$\frac{{{\Gamma }}_{r\text{\_}ie}}{{{\Gamma }}_{n\text{\_}e}}$
with V at several different barrier thickness (c
1 and c
2) cases. (f) The corresponding relationship between
Γ
r
_
i
e
Γ
n
_
e
$\frac{{{\Gamma }}_{r\text{\_}ie}}{{{\Gamma }}_{n\text{\_}e}}$
and P
r
for (d) and (e), respectively. Here, considering the typical electron dephasing time as 10–100 fs [25], we select the best case as 100 fs for the representative, and other electron lifetime cases will be discussed in the next section.](/document/doi/10.1515/nanoph-2023-0231/asset/graphic/j_nanoph-2023-0231_fig_003.jpg)
The breakdown of contraction between high-IQE and large P
r
by mMQW systems. (a) The potential energy and corresponding wavefunctions of mMQWs system. (b) The EVΓ map of the engineered mMQWs system. (c) The EΓ curves under resonant voltages with different c
2. It is worth to note that, by considering the practical fabrication with certain thickness variation, such RIET enhancement from mMQWs may give a relatively lower value (see detailed discussion in Supplementary Material Section 10). (d–e) The variation of
In addition, to gain a more intuitive understanding of how mMQWs can simultaneously achieve high photon-emission power and efficiency, we draw an analogy between the resonant tunneling behavior of electrons and the resonant transmittance behavior of photons in a Fabry–Perot cavity. Generally, for the mMQWs system, the presence of an ultra-strong resonance indicated by a high Q-factor, provides the IQE-improvement basis and promote effective functioning of resonant enhancement realizing both high photon-emission power and efficiency simultaneously (see details in Supplementary Material Section 8). However, one should note that more metal quench and dielectric defects will be induced by adding more layers of MQW, reducing the radiation efficiency of generated photons in mMQW system. Thus, the evaluation of additional loss introduced by the metal quench is performed (see details in Supplementary Material Section 9). The absorption spectrum demonstrates a ∼15–20 % increase as the number of MQW increased from 1 to 3, which has minimal impact on the significant resonant enhancement effect around 1010.
2.3 The IQE and P r with varied electron lifetime
In regarding to practically fabricating the cascaded MQWs system, achieving precise matching of three energy levels under a single bias voltage necessitates high precision in the film processing. Thus, we further discuss the actual device performance with considering the experimental aspects including the effects of thickness variation and defects. Firstly, we investigate the impact of thickness variation on key device parameters. Specifically, when the quantum well thickness deviates by 0.2 nm (approximately one atomic layer), the resonant enhancement factor is reduced from ∼1010 to 107 due to the shift in resonant energy levels (Supplementary Material Section 10). To address this challenge, in addition to the epitaxial growth of single crystal layers, such as TiN and Al2O3 utilized in the present modeling, an alternative approach involves employing a transfer-technique that utilizes two-dimensional materials such as insulating h-BN layers and metallic films [26]. This approach holds promise in meeting the required specifications and enables the construction of a two-dimensional tunneling junction composed of multiple single-crystal monolayers bounded by van der Waals forces. Consequently, the resulting film exhibits ultra-smooth surfaces and precise control over atomic layer thickness, ensuring the desired IQE and photon-emission power [27–29]. Secondly, we investigate the potential impact of defects within the multiple metallic films constituting the device. These defects have the potential to affect the electronic lifetime, with a higher density of defects leading to a shorter electronic lifetime due to increased electron-electron and electron-phonon collisions [30, 31]. Thus, it is necessary to check whether the relationship between

The mMQW system with varied electron lifetime. (a) The variation of
3 Conclusions
In conclusion, we demonstrate that multiple RIET enhanced inelastic electron tunneling events have the potential of eliminating the contraSectdiction between photon-emission power and efficiency. Our proposed three cascaded metallic quantum wells (mMQWs) based tunnel junctions structure is demonstrated to amplify the effect of resonant enhancement, realizing an IQE ∼ 1 and P r ∼ 0.8 µW/µm2 in the best cases with electron lifetime ranging from 10 fs to 100 fs. Theoretically, the performance can be further enhanced by increasing the number of quantum wells, albeit at the expense of more refined fabrication. The proposed structure formed by stacked multilayers can be fabricated straightforwardly by film deposition with high precision [33–36] or by employing transfer-techniques utilizing two-dimensional materials, making it practical for future use in high-efficiency optoelectronic devices. In additional, the maximum emission wavelength range would be tuned by the fermi energy of electrodes. By incorporating high-efficiency optical antennas, we can maximize the external quantum efficiency and enable the realization of quantum light sources in the visible/near-infrared ranges, including single-photon or entangled photons [17], including single-photon or entangled photons [37]. Thus, the implementation of strong RIET-enhanced tunneling structures could open up possibilities for ultra-fast, high-efficiency photon sources for high-performance photonic and plasmonic circuitries.
Funding source: National Natural Science Foundation of China
Award Identifier / Grant number: 62005237
Award Identifier / Grant number: 62175217
Funding source: National Key Research and Development Program of China
Award Identifier / Grant number: 2021YFB2801801
-
Author contributions: H.Q. conceived the idea. Y.Z. conducted the numerical simulations. Y.Z., D.L., S.Z., and H.Q. contributed extensively to the writing of the manuscript. Y.Z., D.L., Y.F., S.Z., and H.Q. analyzed data and interpreted the details of the results. H.C. and H.Q. supervised the research.
-
Research funding: The work at Zhejiang University was sponsored by the National Key Research and Development Program of China under Grant 2021YFB2801801, and the National Natural Science Foundation of China (NNSFC) under Grants No. 62175217, Grants No. 62005237.
-
Conflict of interest statement: The authors declare no competing financial interest.
-
Data availability statement: The datasets generated and/or analyzed during the current study are available from the corresponding author upon reasonable request.
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Supplementary Material
This article contains supplementary material (https://doi.org/10.1515/nanoph-2023-0231).
© 2023 the author(s), published by De Gruyter, Berlin/Boston
This work is licensed under the Creative Commons Attribution 4.0 International License.
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