Resonant four-photon photoemission from SnSe<sub>2</sub>(001)

doi:10.1007/s11467-023-1365-4

Front. Phys.

2024, Vol. 19

Issue (3) : 33207 https://doi.org/10.1007/s11467-023-1365-4

RESEARCH ARTICLE

Resonant four-photon photoemission from SnSe₂(001)

Chengxiang Jiao¹, Kai Huang¹, Hongli Guo², Xingxia Cui¹, Qing Yuan¹, Cancan Lou¹, Guangqiang Mei¹, Chunlong Wu³, Nan Xu³, Limin Cao¹, Min Feng^1,³(

)

¹. School of Physics and Technology and Key Laboratory of Artificial Micro- and Nano-Structures of Ministry of Education, Wuhan University, Wuhan 430072, China
². Department of Physics and Astronomy, California State University Northridge, Northridge, CA 91330-8268, USA
³. Institute for Advanced Study, Wuhan University, Wuhan 430072, China

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Abstract

High-order nonlinear multiphoton absorption is usually inefficient, but can be enhanced by designing resonant excitations between occupied and unoccupied energy levels. We conducted angle-resolved multi-photon photoemission (mPPE) studies on the SnSe₂(001) surfaces excited by ultrashort laser pulses. By tuning photon energy and light polarization, we demonstrate the presence of a resonant four-photon photoemission (4PPE) process involving the occupied valence band (VB), the unoccupied second conduction band (CB2) and the unoccupied image-potential state (IPs) of SnSe₂. In this 4PPE process, VB electrons of SnSe₂ are resonantly excited into CB2 by adsorbing two photons, followed by the adsorption of another photon to populate the n = 1 IPs before being emitted out to the vacuum by adsorbing one more photon. This results in a double-resonant 4PPE process, which exhibits approximately a 40 times enhancement in photoemission yields compared to cases where one of the resonant pathways, CB2 → IPs, is inhibited by involving a virtual state instead of the IPs in the 4PPE. The double-resonant 4PPE process efficiently excite the bulk VB electrons outside the vacuum, like taking advantage of resonant “ladders” through two real empty electronic states of SnSe₂. Our results highlight the important applications of mPPE in probing the band-structure, particularly the unoccupied states, of recently emerging main group dichalcogenide semiconductors. Furthermore, the discovered resonant mPPE process contributes to the exploration of their promising optoelectronic applications.

Keywords multi-photon photoemission four-photon photoemission SnSe₂ unoccupied states resonant excitation

Corresponding Author(s): Min Feng

About author:

Peng Lei and Charity Ngina Mwangi contributed equally to this work.

Issue Date: 22 November 2023

Cite this article:

Chengxiang Jiao,Kai Huang,Hongli Guo, et al. Resonant four-photon photoemission from SnSe₂(001)[J]. Front. Phys. , 2024, 19(3): 33207.

URL:

https://academic.hep.com.cn/fop/EN/10.1007/s11467-023-1365-4
https://academic.hep.com.cn/fop/EN/Y2024/V19/I3/33207

Fig.1 (a) The top and side views of the atomic structure of 1T-SnSe₂. (b) Schematic representation of the 3D Brillouin zones of 1T-SnSe₂ along with its projection onto the (001) surfaces. (c) Typical STM topography image of the SnSe₂(001) surfaces acquired at a sample bias of 0.6 V and a tunneling current of 8 pA. The white rhomboid defines the unit cell of the surface. The atomic structural model of one SnSe₂ sandwich-layer on the surface illustrates that the bright contrast resolved by STM originates from the Se atoms on the top atomic layer. The inset shows typical STS dI/dV spectra acquired on the surfaces.

Fig.2 (a) The normal-emission mPPE spectra versus photon energy measured with p-polarized irradiation from the SnSe₂(001) surfaces. Three separated features, labelled as I, II and III, are marked in the spectra. The insets highlight each of these features individually. (b) The peak positions of features I, II and III in the E_final versus photon energy plot. The dotted line represents the linear fitting of the data for VB, CB2, and IPs. (c) The calculated band structure along K?M?Γ?K of bulk 1T-SnSe₂, relevant to the normal emission geometry of the mPPE. CB2 and VB around Γ point are highlighted red and purple, respectively. (d?g) The 4PPE intensity versus

k / /

along Γ?M with p-polarized incident radiation on SnSe₂ surfaces at different irradiation photon energies. CB2, IPs, and VB are fitted using red, orange and purple parabolic dashed lines, respectively. (h) Schematic representation of band structure alignment at Γ point with the proposed 4PPE resonance for a photon energy near 1.94 eV.

Fig.3 (a) Schematic illustration of the double-resonant 4PPE process of VB → CB2 → IPs → E_final, where the IPs serves as the second intermediate state. (b) Schematic illustration of the VB → CB2 → Vs (virtual state) → E_final 4PPE process, in which the IPs is replaced by a virtual state. In this case, there is no resonance between CB2 with the second intermediate state. (c) The experimental geometry of p- and s-polarized irradiations. s-polarized irradiation contains only the in-plane (

E / / y

) electric field, while the p-polarized light includes both the in-plane (

E / / x

) and out-of-plane (

E ⊥ x y

) components. (d, e) The 4PPE intensity versus

k / /

along Γ?M with p- and s-polarized incident radiation on SnSe₂ surfaces respectively, at a photon energy of 1.94 eV. CB2 and IPs are represented by red and orange parabolic dashed lines, respectively. (f) Normal-emission 4PPE spectra measured with p-polarized (blue) and s-polarized (yellow) irradiations from the SnSe₂ surfaces, corresponding to

k / /

= 0 ?^?1 in (d) and (e), respectively. The spectra are normalized according to the work function edge.

Fig.4 (a?c) The side view of the wavefunction normal (|ψ|²) of VB, CB2, and n = 1 IPs. The parity of |ψ|² is even (+) for VB and odd (?) for CB2 according to the inversion center, as highlighted by the black-dashed rectangle. (d) The calculated transition dipole moment

| T n ′ n i |

(broadened with Gaussian functions) of VB → CB2, CB2 → IPs, and VB → IPs. The energy is relative to E_F.

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